The use of synthetic fibers as reinforcement in fiber-reinforced cementitious composites (FRCC) demonstrates a combination of better ductile response vis-à-vis metallic ones, enhanced durability in a high pH environment, and resistance to corrosion as well as self-healing capabilities. This study explores the effect of macro- and micro-scale polypropylene (PP) fibers on post-crack energy, ductility, and the self-healing potential of FRCC. Laboratory results indicate a significant change in fracture response, i.e., loss in ductility as curing time increases. PP fiber samples cured for 2 days demonstrated ductile fracture behavior, controllable crack growth during tensile testing, post-cracking behavior, and a regain in strength owing to FRCC’s self-healing mechanism. Different mixes of FRCC suggest an economical mixing methodology, where the strong bond between the PP fibers and cementitious matrix plays a key role in improving the tensile strength of the mortar. Additionally, the micro PP fiber samples demonstrate resistance to micro-crack propagation, observed as an increase in peak load value and shape deformation during compression and tensile tests. Notably, low volume fraction of macro-scale PP fibers in FRCC revealed higher post-crack energy than the higher dosage of micro-scale PP fibers. Lastly, few samples with a crack of < 0.5 mm exhibited a self-healing mechanism, and upon testing, the healed specimens illustrated higher strain values.