Molecular hydrogen (H2), methane, and hydrocarbons with an apparent abiotic origin have been observed in a variety of geologic settings, including serpentinized ultramafic rocks, hydrothermal fluids, and deep fractures within ancient cratons. Molecular hydrogen is also observed in vapor plumes emanating from the icy crust of Saturn’s moon Enceladus, and methane has been detected in the atmosphere of Mars. Geologic production of these compounds has been the subject of increasing scientific attention due to their use by chemosynthetic biological communities. These compounds are also of interest as possible energy resources. This issue summarizes the geological sources of abiotic H2 and hydrocarbons on Earth and elsewhere and examines their impact on microbial life and energy resources.