Fiber-reinforced cement composites, particularly those incorporating natural fibers like cellulose, have gained attention for their potential towards more sustainable construction. However, natural fibers present inherent deficiencies in mechanical properties and can benefit from hybridization with carbon fibers. This study focuses on the incorporation of cellulose and carbon fibers, in varying contents, into fibrocement composites, employing a Response Surface Methodology (RSM) to optimize the material characteristics. The methodology involves testing, encompassing flexural tensile, compression, and fracture toughness tests. The results indicate an increasing trend in flexural strength for higher carbon fiber content, peaking near 5%. A plateau in flexural strength is observed between 1.2% and 3.6% carbon fiber content, suggesting a range where mechanical properties stabilize. Compressive strength shows a plateau between 1.2 and 3.6% and reaches its highest value (≈33 MPa) at a carbon fiber content greater than 4.8%, and fracture toughness above 320 MPa·m1/2 is achieved with carbon fiber content above 3.6%. This study offers insights into optimizing the synergistic effects of cellulose and carbon fibers in fibrocement composites.