The process of inclusion of carbon nanotubes as fibers in cement paste has been proved to have optimistic effect as it enhances the tensile property of cement paste composite. Coir fibers have exceptional mechanical qualities and are thus employed as reinforcement in cement composites. Epoxy resin, which has a high Young’s modulus, is an ideal component for bonding carbon nanotubes (CNTs) to coir fiber. This paper describes a novel kind of nanocomposite made of L-12 epoxy resin and CNTs at the nanolevel, along with coir fibers at the microlevel which operate as crack arrestors. To remove surface contaminants, coir fibers are first treated with sodium hydroxide (NaOH). Epoxy/CNTs polymer coatings were developed at varying CNTs fractions (0.05, 0.1, 0.15, and 0.2 wt.% of cement). Multiwalled CNTs were combined in distilled water, followed by epoxy resin and hardener (9 : 1 v/v) polymer in an ultrasonic sonicator for 90 min to ensure full dispersion of CNTs within the epoxy polymer. This blend is now coated on the treated clustered coir fiber (length 10 cm, 10 strands) and reinforced along the length of a cement composite beam 20 mm × 20 mm × 80 mm in size. Tensile and three-point tests were performed to evaluate the mechanical characteristics of the hybrid composite. The linear elastic finite element analysis is employed to distinguish their failure phenomena via fatigue or fracture behavior. The microstructure behavior and the effect of coating material on the coir fibers were investigated using scanning electron microscope and EDX analysis. The reinforcing impact of nanopolymer coated coir fiber in cement composite diminished the tensile and flexural strength after 0.1 wt.% of CNT fraction but increased the composite’s durability and Young’s modulus. Fourier transform infrared spectroscopy analysis was carried out to assess the chemical interaction between the epoxy/CNTs and the coir fibers. The simulation was performed using ANSYS workbench, and the modeling results were within an acceptable 10% range of the experimental data. Nevertheless, it can be concluded that the hybrid composite is capable of enhancing the composite’s stress and strain capacity by regulating the fracture propagation process at the crack’s end.