Nanosilica (NS) has attracted wide variety of usage as cement ingredients. While many other studies have focused on early cement hydration and hardening properties, there is less data available on the impact of NS on the behavior of fiber-reinforced high-volume sugarcane bagasse cement mortar (HVSCBAM). The effects of NS on the fiber-reinforced durability of HVSCBAM, having the properties of sugarcane bagasse ash/binder in an average of 50% by weight, have been presented in detail in this study. Four NS/binder weight ratio dosages of 0%, 0.5%, 1.0% and 1.5% of and another four total PVA fiber/volume ratio dosages of 0%, 0.2%, 0.5% and 1.0% were used. Compared to 0.2-1 vol.% of PVA fiber–reinforced HVSCBAM, the 1.5 wt.% of NS would enhance the compressive strength further. Various reports on mineralogy and microstructure have demonstrated that NS facilitates fiber/matrix bonding. These conclusions provide an insight into the pozzolanic materials of cement that are used in a large volume in the designs and applications of nanoparticles.