The present disclosure relates to methods for making chromium-containing dehydrogenation catalysts using chromium feedstocks that need not include chromium(VI). The disclosure also relates to the catalysts made thereby, as well as to dehydrogenation methods using such catalysts. In one aspect of the disclosure, a method includes providing a formable mixture comprising, on a dry basis, an aluminum hydroxide, present in an amount within the range of about 40 wt. % to about 90 wt. %; an acid (e.g., nitric acid), present in an amount within the range of about 2 wt. % to about 15 wt. %; and a chromium(III) source, present in an amount within the range of about 2 wt. % to about 35 wt. %; forming the formable mixture; and calcining the formed mixture. In certain embodiments, the method further includes impregnating the calcined mixture with an aqueous impregnation solution including a chromium(III) salt; and calcining the impregnated mixture.