The possible reasons that were associated with the reduction of zinc oxide and the deposition of elemental Zn on the zinc-based sorbent surfaces were proposed in this study and examined by monitoring chemical reactivity and physical/chemical properties of the sorbents during the multicyclic tests with the aid of various diagnostics in order to investigate the deactivation of the sorbents that was observed in previous works. The reactivity of the sorbents was investigated using a temperature programmed technique (TPT) with a thermal gravimetric analyzer (TGA). From our experiments, the undesirable features due to the reduction of ZnO that was caused by the reducing components in the gasified coal gas were observed in the chemical reactivity and sorbent properties. In the investigation of the migration of elemental Zn onto the sorbent surface, elemental Zn accumulated on the surface of the sorbents rather than the zinc vaporization. It might have caused the deactivation of the zinc-based sorbents.