In this paper, we report on PbMoO4 crystals grown from melts of controlled stoichiometric variations under different ambient conditions. It is observed that PbMoO4 crystals of different shades not only differ in their impurity contents but their stoichiometries with regard to both cationic and anionic compositions could be different. Annealing studies in air/oxygen as well as in vacuum were carried out on the crystals for a better understanding of the defect centers responsible for the coloration. The role of nonstoichiometric giving rise to coloration is also described. © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.