This study examines the potential of combining tailored binder formulations with engineered polypropylene (PP) fibers to develop a range of Fiber-Reinforced Cementitious (FRC) systems with enhanced ductility and strain-hardening properties, while encompassing sustainability and economic viability. The experimental investigation compares the surface microstructure of novel bicomponent PP fibers, produced using a pilot fiber spinning device, with that of standard PP fibers. Micro-scale single-fiber pull-out tests are conducted to ascertain the extent to which this surface modification contributes to enhanced energy absorption. The effectiveness of these novel fibers at the composite scale is assessed when embedded into two limestone calcined clay cement (LC³) binder systems, in terms of the fresh and hardened properties of the resulting FRLC³, with low cement content (35 % of the total binder). The effect of incorporating super absorbent polymer (SAP) on tailoring the internal porosity of the matrix, thereby promoting the potential for stress transfer via multiple crack pathways, is assessed. A Finite Element Method (FEM) analysis, calibrated with the materials and bond laws retrieved experimentally, is conducted to simulate the tensile and cracking behavior of the optimal material combination investigated in this study, demonstrating a high degree of correlation with the tensile tests.