In light of the well-established multi-scale nature of flaws in concrete, it follows that existing diverse attempts in fiber-reinforced concrete (FRC) technology-intended to mitigate the inherent tendency of concrete to cracking-remain relatively inefficient. This is majorly attributed to the fact that the large inter-fiber spacing in conventionally used macrofibres does not promote an effective bridging of multiscale cracks. As a result, increasing research and development are currently being invested to develop concretes incorporating nanoscale particles. Thus, nanoscale fibers emerged as a promising tool for manipulating concrete nanostructure towards a controlled macrobehaviour necessary for enhanced overall performance. In this context, while carbon nanostructure (CNS) such as carbon nanofibers (CNF) and carbon nanotubes (CNT) have gained a relative popularity, it should be noted that eco-efficiency incentives would favor the currently emerging nanocellulose materials (NCM) extracted from cellulose-based systems, the most abundant and renewable resource on the planet. NCM have been demonstrated as a means to engineer superior composite properties necessary for versatile applications including optics, biomedical applications, and transparent electronics. The current study is aimed at disclosing the possibilities of re-engineering concrete properties using a new type of NCM, namely, cellulose filaments (CF) in order to achieve superior concrete performance necessary for specific applications. CF are cellulosic fibrils with a nanometric diameter (30–400 nm) and micrometric length (100–2000 µm), thereby exhibiting the highest aspect ratio (100–1000) among all currently available NCM. The study focuses on the influence of CF as a tool for nano-tailoring the properties of concrete in its three major states (fresh, hardening, and hardened). As a result, three applications in relation to the above concrete states were identified through intensive experimentation: (i) enhancing the properties of fresh concrete by using CF as a viscosity modifying admixture (VMA), (ii) enhancing the properties of hardening concrete by using CF as a shrinkage reducing admixture (SRA), and (iii) improving the performance of concrete at the hardened state by using CF as a nanoscale reinforcement. The study further aims at leveraging those different enhancements in concrete properties obtained with CF towards developing a new concrete formulation that optimizes the advantages of CF. The enhancement of concrete properties at fresh state was undertaken in the context of valorizing the hydrophilic and flexible nanoscale CF to function as a VMA in self-consolidating concrete (SCC) whereby the design of flowable (yet stable and robust) mixtures requires a delicate balance between flowability and stability. For this, CF were incorporated at concentrations ranging from 0.05 to 0.30% per weight of binder in cement pastes and SCC. CF were demonstrated as a valuable tool not only for rheology modification, but also to impart collateral positive effects on mechanical performance (strength enhancement of 12–26% in compression, splitting-tension, and flexure) when compared to commercially available VMA of Welan Gum type. CF were found to serve as a VMA due to the buildup of flexible nanoscale networks as demonstrated by a geometry-based percolation model as well as by microstructure investigations. Interestingly, this effect was found to be accompanied by a shear thinning effect attributable to the streamlining of flexible nanocellulose fibrils in the direction of flow under increasing shear rates, thereby potentially enhancing pumpability. The potential of CF to enhance the properties of hardening concrete was attempted in the context of exploiting the hydrophilic and hygroscopic characters of CF to mitigate autogenous shrinkage (AS) in ultra-high-performance concrete (UHPC). While s such, when UHPC formulation was adjusted to accommodate CF at rates of 0-0.30% per cement mass, and silica fume content was varied (from 15 to 25%), CF were found to be more beneficial in reducing AS at early-age with a reduction of up to 45% during the first 24 hours and 35% at 7 days. On the other hand, adjusting SF content from 25 to 15% had a negligible effect on AS at early-age (0–4% reduction at 1 day) but a higher effect at later-age (28% reduction at 7 days) attributable to the time-dependent pozzolanicity of silica fume. However, this alternative was found to have adverse effects on mechanical performance (32% lower flexural capacity). Finally, the potential of CF as a nanoscale reinforcement was investigated on cement pastes and on concrete. In the former, strength enhancement in engineering properties (compressive strength, flexural capacity, and elastic modulus) of up to 25% were achieved. In the latter, strength improvements of up to 16% (in compression), 34% (in splitting tension), 22% (in flexure), and 96% (in energy absorption) were obtained. To disclose the mechanisms underpinning the effect of CF on strength of cement systems, the above findings were supplemented by microstructure investigations, namely, degree of hydration and micromechanical properties (indentation modulus M, hardness H, and contact creep modulus C) of major microstructure phases using nanoindentation coupled with quantitative energy-dispersive spectroscopy (NI-QEDS). As a result, the improved macromechanical performance was found to sprout from a twofold microstructure change, i.e.: an increased degree of hydration and higher micromechanical properties of C-S-H gel matrix (~12–25%). To leverage the above different advantages offered by CF on cement and concrete composites, particularly the nanoreinforcing effect and the potential synergy between the nanoscale CF and macrofibers, a novel multi-scale fiber-reinforced strain-hardening cementitious composite (SHCC) was developed. The design of this SHCC followed a new approach that couples packing density optimization with micromechanical tailoring. Thus, high-volume ground-glass pozzolans (HVGP) were incorporated under the guidance of particle pacing optimization to replace fly ash (FA) commonly used in SHCC such that composite strength can be increased. The newly formulated SHCC was further improved in terms of ductility and strain-hardening capacity by the incorporation of CF whereby the latter was a useful tool to nanomodify SHCC matrix and interface properties towards enhanced strain-hardening behavior. In outcome, HVGP-SHCC formulations with GP replacement of fly ash of up to 100% were developed. The resulting formulations have self-consolidation ability (mini-slump dimeter in the range of 250 mm) and exhibited (at 28 days) 60-75 MPa compressive strength, 9-15 MPa flexural capacity, 3-6 MPa tensile strength, 2-5% tensile strain capacity, and a significantly increased electrical resistivity (up to 60% enhancement). Thus, the mechanical properties of the newly developed HVGP-SHCC exceed those reported in the commonly used high-volume fly ash (HVFA)-SHCC. Nevertheless, while the strength enhancement obtained with GP does not jeopardize composite ductility up to 40% GP content, a reduced ductility was noticed at GP>40%. As a result, CF were used to impart a nanoreinforcing effect to HVGP-SHCC as well as to nanomodify the interface properties of PVA fibers. In outcome, a twofold effect was obtained by nanomodifying SHCC with CF: (i) CF imparted higher elastic modulus to the bulk cementitious matrix (Em) thereby contributed to attenuating the crack tip toughness (J_tip=K_m^2/E_m) with Km being matrix fracture toughness, (ii) CF led to attenuating the excessive frictional bond encountered at higher GP content (densifying the matrix and increasing its strength, but limiting strain-hardening behavior) and imparted a characteristic slip-hardening effect (β) which contributed towards improving composite strain-hardening capacity and ductility. Thus, enhancement in ultimate strain-capacity above 200% as compared to systems without CF were obtained. Therefore, with the incorporation of CF, it was possible to produce SHCC with up to 100%GP replacement of FA while exhibiting higher strength and ductility. To scale-up the enhanced mechanical performance (particularly the high strength and ductility) demonstrated by the new SHCC, the latter was used as a topping to develop a novel type of composite deck slabs at full-scale (dimensions of up to 2400 × 900 mm). The composite deck slabs thus constructed are intended to benefit from the improved strength and ductility of nanomodified HVGP-SHCC topping such that better compatibility between the steel deck and its concrete topping can be obtained. This has the potential to increase the performance of composite deck slabs under shear bond failure, a major failure mode in composite deck slabs. Results indicated that, compared to composite deck slabs with a high-strength concrete topping having similar compressive strength as the nanomodified HVGP-SHCC, the slabs constructed with the SHCC exhibited up to 35 and 42% enhancement in ultimate load-carrying capacity and ductility, respectively. Furthermore, composite deck slabs with nanomodified HVGP-SHCC exhibited higher shear bond capacity. Considering theses results, it is perceivable that the newly developed SHCC (implemented from the material level at the nanoscale to the structural level at the macroscale) has benefited from a twofold ecoefficiency perspective. The first concerns the valorization of post-consumer recycled glass into the development of high-performance concrete, thereby contributing to relieve a significant socio-economical burden created by landfilling post-consumer glass. The second concerns exploiting the power of cellulose, the most abundant naturally occurring polymer on the planet, towards a biomimetic design of high-performance multiscale-reinforced cement composites necessary for sustainable and resilient concrete infrastructure systems.