The ZnO-MoO3 phase diagram in the range of ZnO compositions from 0.95 to 1.05 mol % is refined by differential scanning calorimetry. Data on crystal stoichiometry are obtained using the weighting method by reducing ZnMoO4 in a hydrogen atmosphere. The specific features of solid-phase synthesis of ZnMoO4 are studied, and its heat of fusion is measured. The modes of solid-phase synthesis and growth of ZnMoO4 crystals are optimized. Some experimental data on the ZnMoO4 crystal growth in the  direction by the low-thermal gradient Czochralski method are presented. Crystals with a cross section of ∼50 × 50 mm2, a length of 160 mm, and a weight up to 1 kg have been obtained.