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Large flawless crystals of ZnO up to 25×10×5 mm3 in size have been grown hydrothermally in a specially designed autoclave. Difficulties on the hydrothermal growth of ZnO single crystals were almost surmouted by in situ determination of solution temperatures under operating conditions. The characteristics of the growth crystals are discussed on the basis of the correlation with growth conditions, and it is found that a nonstoichiometry in the grown ZnO is enhanced with being apt to involve O vacancies due to a reductive atomosphere under hydrothermal conditions and also is related to their some properties.