High levels of naturally occurring arsenic are found in the shallow reducing aquifers of West Bengal, Bangladesh, and other areas of Southeast Asia. These aquifers are used extensively for drinking water and irrigation by the local population. Mechanisms for its release are unclear, although increasing evidence points to a microbial control. The type of organic matter present is of vital importance because it has a direct impact on the rate of microbial activity and on the amount of arsenic released into the ground water. The discovery of naturally occurring hydrocarbons in an arsenic-rich aquifer from West Bengal provides a source of potential electron donors for this process. Using microcosm-based techniques, seven sediments from a site containing naturally occurring hydrocarbons in West Bengal were incubated with synthetic ground water for 28 d under anaerobic conditions without the addition of an external electron donor. Arsenic release and Fe(III) reduction appeared to be microbially mediated, with variable rates of arsenic mobilization in comparison to Fe(III) reduction, suggesting that multiple processes are involved. All sediments showed a preferential loss of petroleum-sourced n-alkanes over terrestrially sourced sedimentary hydrocarbons n-alkanes during the incubation, implying that the use of petroleum-sourced n-alkanes could support, directly or indirectly, microbial Fe(III) reduction. Samples undergoing maximal release of As(III) contained a significant population of Sulfurospirillum sp., a known As(V)-reducing bacterium, providing the first evidence that such organisms may mediate arsenic release from West Bengali aquifers.