This contribution presents the results of profile in-situ gamma spectrometry measurements that sought to determine the content of natural radionuclides ⁴⁰K, ²³⁸U and ²³²Th in a near surface horizon of rocks, their weathering cover and soils in the area of the Malé Karpaty Mts. It is widely established that the exploration of radioactivity of bedrocks and cover rocks can be a very effective and useful tool for both geological mapping, for identifying deposits of mineral resources, and even addressing the issues of structural and tectonic geology. This assertion is equally confirmed by the ground gamma spectrometry measurements carried out as part of this case study on larger scales, seeking more detailed geological structure solutions. The results obtained provide a welcome addition to an already existing database, which monitors the content of naturally occurring radionuclides individually for every rock lithotype of the Western Carpathians, by elaborating on the data collected by previous research and by updating this database for any future needs. The presented results confirmed the low to medium radioactivity levels of rocks and soils in the studied area. The highest values were detected in granitoids and metamorfic phyllitic rocks of the Malé Karpaty Mts. core; the lowest values were detected in carbonates, arenaceous sediments and, above all, amphibolite bodies. In this way, the presented results of the interpreted profile (P5) confirm the model of local geological structure as represented on the most up-to-date edition of the geological map of the Malé Karpaty Mts. (Polák et al. 2011).