We present methane data from along the coast of Barter Island, Alaska, collected with an Unmanned Aerial System and an off-the-shelf, cost-effective methane sensor. The data were collected on September 3 and September 5, 2017, as part of a larger Arctic coastal erosion investigation study by the U.S. Geological Survey (USGS). The data contain latitude, longitude and CH4 (ppm), and are presented as tab-delimited text files that have been zipped into one file. In addition, we have included one file of comparative data from Barrow, Alaska that were collected by the National Oceanic and Atmospheric Administration (NOAA) Global Monitoring Division from 1986-2017 as a courtesy to users. The three datasets together accompany Oberle, F.K.J., Gibbs, A.E., Richmond, B.M., Erikson, L.H., Waldrop, M.P., and Swarzenski, P.W., 2019, Towards determining spatial methane distribution on Arctic permafrost bluffs with an unmanned aerial system: SN Applied Sciences, https://doi.org/10.1007/s42452-019-0242-9.