Methane (CH4) in the subsurface ocean is often supersaturated compared to equilibrium with the modern atmosphere. In order to investigate sources of CH4 to the subsurface ocean, isotope surveys (14C-CH4, δ13 C-CH4, δ2 H-CH4) were conducted at five locations: Skan Bay (SB), Santa Barbara Basin (SBB), Santa Monica Basin (SMB), Cariaco Basin (CB), and the Guaymas Basin (GB). Depth distributions of CH4 concentration and isotopic abundance were determined for both the sediment and water column at the SB, SBB, SMB, and CB sites; CH4 emitted from seeps on the continental shelf adjacent to the SBB as well as seeps and decomposing clathrate hydrates in the GB was also collected, purified, and analyzed. Methane isotope distributions in the sediments were consistent with known methanogenic and methanotrophic activity; seep- and clathrate-hydrate-derived CH4 was found to be depleted in radiocarbon. However, surprising results were obtained in the water column at all sites investigated. In SB the radiocarbon content of the subsurface CH4 concentration maximum was on average 41% less than its suspected sediment CH4 source, suggesting CH4 seepage in the bay. In the SBB, SMB, and CB, the 14C-CH4 contents in the subsurface ocean were 1.2 to 3.6 times greater than modem carbon quantities suggesting a source of 14C from atmospheric nuclear weapons testing, nuclear power plant effluents, or cosmogenic isotope production. Copyright 2008 by the American Geophysical Union.