Sponge gourd (Luffa cylindrica L.) fiber-reinforced cement composites were developed and analyzed. Dried sponge gourd fruit’s fibrous vascular system forms a natural 3D network that can reinforce matrices in composite materials, diverting cracks along the complex array of 3D interfaces between the fibers and the cementitious matrix. To avoid fiber deterioration, the cement paste was modified by incorporating pozzolanic materials. The fibers were mechanically characterized by tensile testing of strips of the 3D natural fiber array and of single fibers extracted from the array. The fibers had an average tensile strength of 140 MPa and an average Young’s modulus up to 28 GPa. Image analysis showed that the fiber spatial distribution inside the 3D network was random. The modified cement paste was characterized by its workability (flow table test) and mechanical behavior (compression and three-point bending tests), with average results of 430 mm, 62.7 MPa, and 6.2 MPa, respectively. Under bending, the cement matrix collapsed after the first crack. The sponge gourd-cement composite manufactured with 1 wt% of fibers showed an average flexural strength of 9.2 MPa (approximately 50% greater than the unreinforced matrix). Importantly, the composite also presented a limited deflection-hardening behavior. These results support sponge gourd’s possible use as reinforcement in cement matrix composites.