ZrMo2O8 was synthesized via two routes, namely, the traditional solid-state method and the solution combustion method. The compounds were characterized by powder X-ray diffraction, UV-visible spectroscopy, scanning electron microscopy, and transmission electron microscopy. The crystals belong to a trigonal crystal system, space group P3̄1c (No. 163) with a = 10.1391(6) Å, c = 11.7084(8) Å, and Z = 6. The band gap of the compounds was around 2.7 eV, and DFT calculations suggest the indirect nature of the band gap. The irregular MoO4 tetrahedra create a dipole and inhibit the process of electron - hole recombination, thereby making the material photoactive. The photocatalytic activity of the compounds prepared by both routes has been investigated for the degradation of various dyes under UV irradiation, and this showed the specificity of the compounds towards the degradation of non-anthraquinonic dyes. © 2009 American Chemical Society.