Endowing dental resin composites (DRCs) with suitable radiopacity is necessary for clinical diagnosis during treatment of caries. To reach this effect, ZrO 2 nanoparticles were introduced into the DRCs in this work after modification with two different methods, one modified with 3-methacryloxypropyltrimethoxysilane (ZrO 2 @γ-MPS) and the other coated with mesoporous SiO 2 and then modified with γ-MPS (ZrO 2 @m-SiO 2 @γ-MPS). These ZrO 2 nanoparticles were used as functional additives, and the SiO 2 nanoparticles were used as the fundamental filler in the preparation of DRCs to study the effects of the surface modification of ZrO 2 nanoparticles and the amount of particles added (0, 3, 5, and 7 wt %) on the properties of the DRCs. The DRC containing ZrO 2 @m-SiO 2 @γ-MPS showed a higher transmittance, which may be attributed to the fact that the SiO 2 coating reduced the refractive index of the nanoparticles and thus decreased the scattering of light within the DRC. The silane polymer film on the surface of ZrO 2 @γ-MPS nanoparticles acted as a lubricant and decreased the viscosity of DRC, but the DRC containing ZrO 2 @m-SiO 2 @γ-MPS showed a higher viscosity due to the presence of a mesoporous structure. The radiopacity value of the DRCs containing the functional additives was close to 1 mm Al, much higher than that of the DRC filled with SiO 2 nanoparticles alone (0.74 ± 0.07 mm Al), meeting the requirement of ISO 4049:2009. The surface modification of ZrO 2 nanoparticles had no significant influence on the mechanical properties, radiopacity, and cytotoxicity of DRCs (p > 0.05). This study provides useful insight into the design and development of radiopaque DRCs with excellent physical and mechanical properties.