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Abstract The catalytic oxidative dehydrogenation of propane (ODHP) is a challenging reaction due to facile competing overoxidation to CO_x. The gaseous disulfur molecule, S₂, is isoelectronic with O₂and has been shown to act as an alternative, “soft oxidant” for the analogous process (SODHP) over bulk metal sulfide catalysts. However, these bulk catalysts suffer from low surface areas and ill‐defined active sites – issues that might be addressed with a supported catalyst. Here we investigate supported V/Al₂O₃materials for SODHP. We show that these catalysts are highly selective for propylene, far surpassing the yields of the prior bulk systems. Isolated sulfided vanadium species are found to be more active and selective than crystalline vanadium sulfide. Additionally, we compare the S₂and O₂oxidants over sulfided and calcined V/Al₂O₃materials, respectively, and find that the propylene selectivity is enhanced using S₂as the oxidant. These results suggest that sulfur is a promising soft oxidant that can be used to achieve high propylene selectivities over supported metal sulfides.