Photocatalytic and photophysical properties of CaZrTi2O7 were investigated. When the CaZrTi2O7 powder was prepared by a polymerizable complex method in the presence of Cs2CO3 flux, powder with high crystallinity and 100-300 nm of a primary particle size was obtained. The band gap of the CaZrTi2O7 powder was 3.6 eV. It showed a broad photoluminescence band around 580 nm at 77 K. Activated NiO/CaZrTi2O7 showed photocatalytic activity for water splitting into H-2 and O-2 under UV irradiation.