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SiO2-poly(2-hydroxyethyl methacrylate) (pHEMA)-based composites have been widely used as biomaterials owing to their biocompatibility. However, they have not yet been applied as tooth restorative materials because of their poor mechanical properties. In the present paper, we develop a novel SiO2/pHEMA-based composite with a polymer-infiltrated network (PICN) structure for use in dental restorative materials. A mixture of SiO2 nanoparticles and a poly(vinyl alcohol) binder was sintered at 950 °C to fabricate a porous SiO2 block. A monomer mixture containing 70 wt%-HEMA/30 wt%-ethylene glycol dimethacrylate and a benzoyl peroxide initiator was infiltrated into the porous SiO2 block and heat-polymerized to fabricate the SiO2/pHEMA-based composite with a PICN structure. The composite was characterized according to its mechanical properties, surface free energy, and bonding properties with a dental adhesive. The flexural strength was 112.5 ± 18.7 MPa, the flexural modulus was 13.6 ± 3.4 GPa, and the Vickers hardness was 168.2 ± 16.1, which are similar values to human teeth. The surface free energy of the polar component of the composite was 19.6 ± 2.5 mN/m, suggesting that this composite has an active surface for bonding with the adhesive. The composite bonded well to the adhesive, in the presence of a silane coupling agent. The SiO2/pHEMA-based composite was demonstrated to be a potential candidate for dental restorative materials.