The increasing environmental concerns about synthetic polymers as reinforcement in the construction industry have highlighted the need for eco-friendly, biodegradable fibers as potential alternative materials for cementitious composites. This study examines the influence of chitosan particle concentrations on the midterm compressive strength of mortars. Chitosan particles, derived from shrimp shells, were mixed with high early strength hydraulic cement at various percentages (0, 0.05, 0.25, 0.5, 1, and 2 wt %) and silica sand to prepare the mortar samples. The findings indicate that chitosan affects the hydration process through the distribution of chitosan particles within the mortar matrix and slightly improved midterm mechanical properties. A life cycle assessment (LCA) revealed a slight increase in greenhouse gas emissions and embodied energy for chitosan-modified mortars, likely due to the use of chemicals in the chitosan synthesis and purification process. In fact, the addition of 0.25 wt % of chitosan into the mortar only added 1.3% of the global warming potential of the sample when compared to the control sample. Incorporating chitosan into a mortar matrix does not significantly affect the resistance-mechanical properties of the composite. The hydration of the cement mortar appears to be slowed by the inclusion of chitosan particles in the cementitious matrix. This research lays the groundwork as one of the first studies for the development of high-performance, early strength cement using chitosan, contributing to a more sustainable construction industry.