Geologic materials are a potential source of external gamma radiation in buildings due to the presence of radioisotopes ( 40 K and isotopes from U and decay families). e contents of these radioisotopes can be evaluated by laboratory analyses that require the extraction of samples, with associated financial and time constraints, and it is also difficult to perform on materials already applied in existing structures. In this work, portable gamma spectrometry results are compared with laboratory analyses in terms of radioisotopes estimations, and the activity concentration index is calculated from them (which assess the conjoint contribution of the different radioisotopes to the external gamma radiation). e studied objects are rocks and their "in situ" weathering products.e results obtained indicate that despite several problems posed by field measurements with portable gamma spectrometry, namely, in terms of the geometric characteristics of the objects measured, this technique has the potential to identify materials with different hazard levels related to external gamma radiation.