The ability of specialist prokaryotes to couple the oxidation of organic compounds to the reduction of Fe(III) is widespread in the subsurface. Here microbial Fe(III) reduction can have a great impact on sediment geochemistry, affecting the minerals in the subsurface, the cycling of organic compounds and the mobility of a wide range of toxic metals and radionuclides. The contamination of the environment with radioactive waste is a major concern worldwide, and this review focuses on the mechanisms by which Fe(III)-reducing bacteria can affect the solubility and mobility of one of the most common radionuclide contaminants in the subsurface, uranium. In addition to discussing how these processes underpin natural biogeochemical cycles, we also discuss how these microbial activities can be harnessed for the bioremediation of uranium-contaminated environments.