The present invention relates to methods for producing metal-supported thin layer skeletal catalyst structures, to methods for producing catalyst support structures without separately applying an intermediate washcoat layer, and to novel catalyst compositions produced by these methods. Catalyst precursors may be interdiffused with the underlying metal support then activated to create catalytically active skeletal alloy surfaces. The resulting metal-anchored skeletal layers provide increased conversion per geometric area compared to conversions from other types of supported alloy catalysts of similar bulk compositions, and provide resistance to activity loss when used under severe on-stream conditions. Particular compositions of the metal-supported skeletal catalyst alloy structures can be used for conventional steam methane reforming to produce syngas from natural gas and steam, for hydrodeoxygenation of pyrolysis bio-oils, and for other metal-catalyzed reactions inter alia.