This data set contains archival raw, partially processed, and ancillary/supporting radio science data acquired during the Gravity Recovery and Interior Laboratory (GRAIL) mission. The radio observations were carried out using the twin GRAIL spacecraft and Earth-based receiving stations of the NASA Deep Space Network (DSN). The observations were used in generating high-resolution gravity field models of the Moon. Of most interest are likely to be the Orbit Data Files in the ODF directory, the Radio Science Receiver files in the RSR directory, and the ionospheric and tropospheric media calibration files in the ION and TRO directories, respectively. The data set includes all raw radio science data collected in the course of the GRAIL mission (September 2011 - December 2012).