Functional hybrid materials were successfully synthesized from low-cost waste products, such as oligochitosan (OCS) obtained from chitosan (one of the main components in crab shells) and nanosilica (nSiO2) obtained from rice husk, in a 1:1 ratio (w/w), and their dispersion in the presence of carboxymethyl cellulose at pH 7 was stable for over one month without aggregation. The molecular weights, chemical structures, morphologies, and crystallinities of the obtained materials were characterized by GPC, FTIR, TEM, and XRD, respectively. The antifungal effects of OCS, nSiO2, and the OCS/nSiO2 hybrid materials were investigated via a disk-diffusion method. The results showed that the nanohybrid materials had better resistance to Phytophthora infestans fungus than the individual components, and a concentration of the OCS2/nSiO2 hybrid material of 800 mg L−1 was the lowest concentration where the material completely inhibited Phytophthora infestans growth, as measured via an agar dilution method. This study not only creates a novel environmentally friendly material with unique synergistic effects that can replace current toxic agrochemicals but also can be considered a new platform for further research in green agricultural applications.