This paper investigates the mechanical properties and the durability implications of innovative cement-based mortars doped with carbon microfibers. In particular, mixes with different amounts of carbon additions are produced, and the properties of fresh and hardened samples are analyzed through workability, water absorption, and compressive and flexural tests under specific environmental conditions. These composites can be employed to enhance construction performance or provide structures with strain-monitoring capabilities. However, the analysis of their mechanical properties and their durability behavior is needed before extensive structural use. In this work, the preparation procedure is defined for the various mix designs, considering different amounts of carbon microfibers; then, fresh properties are evaluated, and different types of samples formed. After various curing times, the specific rheological and hardened properties of the specimens are tested in different conditions to consider the durability of the composites, essential for the real-scale adoption in structural elements. Preliminary electrical and sensing tests are first conducted to evaluate the monitoring potential of the investigated composites. The findings highlight the impact of carbon inclusions on the performance of cement-based mortars, offering valuable insights for their utilization in masonry construction or for repairing concrete structures. In particular, sensing capabilities are found to be highly enhanced by the presence of CMF. Additionally, the results of this research pinpoint key areas for further analysis in the material’s development process.