Cetyl trimethyl ammonium bromide (CTAB)-modified natural rubber latex/Portland cement paste (CTAB + NL/PC) composites were fabricated by varying the NL/cement and CTAB/cement ratios to improve the elastic property of PC. The stability and workability of the CTAB-modified NL particles in the PC matrix were significantly improved. The microstructure and dielectric property analyses of PC, CTAB/PC, NL/PC, and (CTAB + NL)/PC composites were performed to describe the interaction mechanism between the CTAB-modified NL and PC. The portlandite phase in PC was reduced by incorporating CTAB + NL. Although the tensile strength of NL/PC was significantly increased, its compressive strength also greatly decreased by ~40.3%. The tensile and compressive strengths of CTAB/PC were not significantly improved. Notably, the tensile strength of (CTAB + NL)/PC was significantly increased compared to those of PC, CTAB/PC, and NL/PC, while the depreciated compressive strength was only 18.7%. The optimized compressive–tensile performance of (CTAB + NL)/PC was equal to that of PC. The dielectric constants of NL/PC, CTAB/PC, and (CTAB + NL)/PC were reduced due to the low dielectric constant of NL and the ability of CTAB to capture negative charges in the PC matrix, leading to a reduction in the negative surface charges and hence the interfacial polarization. This result was confirmed by the decreased loss tangent in a low-frequency range, which is usually reduced by decreasing the free charges. This work provides a comprehensive guideline for significantly improving the elastic property of PC while retaining a high compressive strength.