Zinc oxide-based sorbents, and processes for preparing and usingthem are provided, wherein the sorbents are preferably used toremove one or more reduced sulfur species from gas streams. Thesorbents contain an active zinc component, optionally incombination with one or more promoter components and/or one or moresubstantially inert components. The active zinc component is a twophase material, consisting essentially of a zinc oxide (ZnO) phaseand a zinc aluminate (ZnAl.sub.2 O.sub.4) phase. Each of the twophases is characterized by a relatively small crystallite size oftypically less than about 500 Angstroms. Preferably the sorbentsare prepared by converting a precursor mixture, containing aprecipitated zinc oxide precursor and a precipitated aluminum oxideprecursor, to the two-phase, active zinc oxide containingcomponent.