The preparation of novel polymeric dental restorative materials (PDRM) was carried out using hybrid-filler, which was consisted of fumed silica microfiller and barium glass macrofiller, resulting in the improvement of mechanical properties of PDRM. In order to enhance the miscibility of inorganic hybrid-filler with organic resin matrix in PDRM and to conduct the homogeneity of filler, its surface was hydrophobically treated with γ-methacryloxypropyl trimethoxysilane and freeze-drying method was adopted to remove the solvents. Diametral tensile strength, flexural strength, Knoop hardness, polymerization shrinkage, and abrasion resistance of PDRM prepared were investigated comparing with those of commercial PDRM products. The PDRM produced in this work showed excellent mechanical properties as well as superior polymerization shrinkage values. It was also discovered that PDRM prepared by using hybrid-filler resulted in better surface characteristics.