We have completed a mapping study of 7.6 MeV gamma rays produced by neutron capture by Fe at the surface of the main belt asteroid 4 Vesta as measured by the bismuth germanate scintillator of the Gamma Ray and Neutron Detector (GRaND) on the Dawn spacecraft. The procedures used to determine Fe counting rates are presented, along with a global map, constituting the necessary initial step to quantify Fe abundances. While the final calibration of orbital data to absolute concentrations has not been determined, the range of fully corrected Fe counting rates is compared with that of Fe in howardites. We find that the global distribution of corrected Fe counting rates is generally consistent with mineralogy and composition determined independently by other instruments on the Dawn spacecraft, including measurements of pyroxene absorption bands by the Visible and Infrared Spectrometer and Framing Camera, and an index of diogenitic materials provided by neutron absorption measurements by GRaND. In addition, there is a distinctive low Fe region in the western hemisphere that was not reported by reflectance or optical observations, possibly indicating the presence of a cumulate eucrite component in Vesta's regolith.