Nanoparticulate Cd1−xZnxO (x = 0, 0.05–0.26, 1) is synthesized in a simple two-step synthesis approach. Vapor-diffusion induced catalytic hydrolysis of two molecular precursors at low temperature induces co-nucleation and polycondensation to produce bimetallic layeredhydroxide salts (M = Cd, Zn) as precursor materials which are subsequently converted to Cd1−xZnxO at 400 °C. Unlike ternary materials prepared by standard co-precipitation procedures, all products presented here containing < 30 mol% Zn2+ ions are homogeneous in elemental composition on the micrometre scale. This measured compositional homogeneity within the samples, as determined by energy dispersive spectroscopy and inductively coupled plasmaspectroscopy, is a testimony to the kinetic control achieved by employing slow hydrolysis conditions. In agreement with this observation, the optical properties of the materials obey Vegard's Law for a homogeneous solid solution of Cd1−xZnxO, where x corresponds to the values determined by inductively coupled plasma analysis, even though powder X-ray diffraction shows phase separation into a cubic mixed metal oxide phase and a hexagonal ZnO phase at all doping levels.