The flexural strength and compressive strength are the two most important parameters that characterize the mechanical properties of cement-based materials, but the two are usually mutually exclusive or negatively correlated. The flexural strength of cement-based materials cannot be effectively improved by a single nano -material without reducing their compressive properties. Therefore, compounding various micro-nano materials, fully utilizing their respective advantages, and developing composite materials with new properties and appli-cation characteristics are important techniques for enhancing the mechanical properties of cement-based ma-terials. This study aimed to investigate the synergistic enhancement of the mechanical properties of concrete by using microcrystalline cellulose (MCC) and nano-silica (NS) composites. MCC and NS were mixed and modified to synthesize MCCNS materials, which were added to cement slurry for experiments. Results indicated that the flexural strength and compressive strength of the cement paste with MCCNS materials were significantly increased compared with those of the cement pastes without MCCNS or with only NS. The flexural strength of the cement paste with MCCNS-1 was increased by 47%, 20%, 6.3%, and 6.8% after curing for 1, 7, 28, and 56 days, respectively. Meanwhile, compressive strength was also increased by 14.4%, 6.3%, 6.8% and 6.5%, respectively. In addition, the reaction mechanism was speculated through a variety of test results. The addition of MCCNS material facilitated the formation of additional C-S-H, which also contributed to enhancing the mechanical properties of cement paste.