As a continuation of efforts to explore the potential of certain types of polymer nanocomposites to be successful candidates as dental restoration/adhesion materials, a Zr‐containing and organically modified silicate‐based material system with epoxy functionality was prepared by use of a sol–gel synthesis method, and UV light‐ and visible light (VL)‐curing processes. Comparative influences of the synthesis and processing parameters on the mechanical, thermal, and microstructural/nanostructural properties of the system were detailed. Zr‐containing species proved to more effectively catalyze the epoxy polymerization/crosslinking reactions than those containing Ti. Incorporation of Zr into the nanocomposite network led to significantly advanced mechanical properties. An elastic (Young's) modulus value of 23 MPa was achieved. The system with relatively high Zr content was successfully obtained, which also had higher thermal stability. Overall observations and results suggested that Zr content, and the UV light‐ or VL‐curing process could be capitalized on to modify the structure, and to improve the final properties of these material systems, which indicated a prospective opportunity for this material system to be utilized in dental restoration/adhesion applications. POLYM. ENG. SCI., 55:792–798, 2015. © 2014 Society of Plastics Engineers