This paper reports new hierarchical cementitious composites developed using microcrystalline cellulose (MCC), sisal fibers and cetyltrimethylammonium bromide (CTAB) as the dispersing agent. MCC was dispersed in water without and with CTAB at different concentrations using ultrasonication and the optimum CTAB concentration for achieving homogeneous and stable MCC suspensions was found to be 40%. Hierarchical composites were fabricated using MCC (0.1–1.5 wt% of cement), sisal fibers (20 mm, 0.25% and 0.50 wt% of cement), 40% CTAB and tri-butyl phosphate as the defoaming agent. Mechanical strengths of composites improved significantly at 0.1 wt% MCC, which along with 0.5% sisal fibers improved compressive and flexural strengths by ~ 24% and ~ 18%, respectively. The hybrid reinforcement exhibited a synergistic effect on the fracture behavior of composites improving the fracture energy up to 40%. Hierarchical composites also showed improved fiber-matrix bonding, lower porosity and water absorption, superior hydration, carbonation resistance and durability up to 90 ageing cycles.