ZnTiO₃ was synthesized by sol–gel processing using a single-source precursor in which the two metal atoms are linked by means of p-carboxybenzaldehyde oxime. According to spectroscopic investigations, the COOH group is coordinated to Zn²⁺ and the oximate group to a Ti(OiPr)₃ moiety. The temperature-dependent structure evolution of ZnTiO₃ was investigated to illustrate the advantage of this approach compared to materials prepared from two individual precursors (zinc benzoate and oximate-modified Ti(OiPr)₄). ZnTiO₃ prepared from the single-source precursor has a more homogeneous structure through all stages of the synthesis process and a higher surface area. The latter results in a higher activity in the photocatalytic degradation of methylene blue.