Zinc oxide-based sorbents, and processes for preparing and using them are provided, wherein the sorbents are preferably used to remove one or more reduced sulfur species from gas streams. The sorbents contain an active zinc component, optionally in combination with one or more promoter components and/or one or more substantially inert components. The active zinc component is a two-phase material, consisting essentially of a zinc oxide (ZnO) phase and a zinc aluminate (ZnAl2O4) phase. Each of the two phases is characterized by a relatively small crystallite size of typically less than about 50 nm (500 Angstroms). Preferably the sorbents are prepared by using an alkali metal base to convert a precursor mixture, containing a precipitated zinc oxide precursor and a precipitated aluminum oxide precursor, to the two-phase, active zinc oxide containing component, with the resulting sorbent having a sodium level within a desired range.