Coupled gamma-ray spectrometric and lithogeochemical studies throughout the Heath Steele Mines area, Bathurst Camp, New Brunswick, indicate that primary and secondary geochemical differences exist between the stratigraphic footwall and hangingwall crystal tuff units which host the massive sulfide deposits. Of particular interest is Th, and to a lesser extent, Zr and Y, which are more concentrated in the hangingwall than the footwall crystal tuffs, whereas the opposite is true for TiO 2 . This expands on earlier lithogeochemical-chemostratigraphic results concentrated in the eastern part of the Heath Steele belt that led to revision of the local stratigraphy, and necessitated a structural re-interpretation of the area with implications for exploration. Although K depletion (decreased K and K/Th) is typical of chloritized footwall zones of chloritization, these features were not fully apparent here due to the recessive nature of these altered zones. In situ radiometric analysis using a portable gamma-ray spectrometer is a rapid, inexpensive analytical technique for chemostratigraphic characterization of rock units within volcanogenic massive sulfide deposit settings, provided there is a contrast in the distribution of natural radioelements, particularly Th and K.