AseriesofxNiAl2O4/γ-Al2O3compositeswithvariousNicontentshavebeenpreparedviaone-steppartialhydrolysisofmetalnitratesaltsintheabsenceofsurfactantsandusedforcarbondioxidereformingofmethane.ThecharacterizationresultsdemonstratedthattheNiAl2O4/γ-Al2O3materialspossessedmesoporousstructuresofuniformporesizes;andtheNi2+ionswerecompletelyreactedwithaluminatoNiAl2O4spinelinthematricesusingN2sorption,XRD,TEM,andXPS.TheNiAl2O4/γ-Al2O3materialsexhibitedexcellentcatalyticpropertiesandsuperiorlong-termstabilityforcarbondioxidereformingofmethane.TheeffectsofNicontentontheintrinsicactivitiesandtheamountsofcokedispositionofthexNiAl2O4/γ-Al2O3catalystswerediscussedindetailforthecarbondioxidereformingofmethane.TheresultsrevealedthattheNiparticlesizesdidnotaffecttheintrinsicactivityofmetallicNi,butsmallerNiparticlescouldreducetherateofcokedeposition.