Comparing different synthesis methods to investigate ambient degradation differences among ZnO crystals with different crystal habits, we examined the effects of particle size, surface area, shape (surface polarity), and zeta (surface) potential. Neither surface polarity nor surface area, on their own, can account for the differences in the surface carbonation among differently synthesized ZnO samples. Our results demonstrate that surface dissolution and carbonation tendencies must be considered together, in the context of surface polarity, to explain different propensities toward degradation in ZnO powders.