The spin coherence time (T2*) in ZnO single crystals at 8.5 K decreases significantly from ∼11.2 ns to ∼2.3 ns after annealing at 500 °C, as indicated by time-resolved Kerr-rotation pump-probe magneto-optical spectroscopy. The annealing-induced spin coherence degradation in ZnO arises neither from crystallinity degradation during the annealing process, as confirmed by x-ray rocking curves; nor from reflection variations of the probe laser beam induced by surface roughness changes during the annealing process, as confirmed by atomic force microscopy. Temperature-dependent Hall-effect studies indicate that decreased mobility and increased shallow-donor concentration in the annealing-induced surface conducting layer on top of the bulk ZnO are most likely to be the reasons for the spin coherence degradation in ZnO during the annealing process.