This pioneering study investigated the activity concentrations of naturally occurring radionuclides in 25 quarry pit soils collected from Jhalokati, Barishal, and Dhamrai, Bangladesh. HPGe γ-ray spectrometry revealed that the measured activity concentrations of 226Ra (15–22 Bq/kg), 232Th (14–34 Bq/kg), and majority of 40K (260–480 Bq/kg) in quarry pit soils were below the worldwide average values of 30, 35, and 400 Bq/kg, respectively. Importantly, 137Cs was undetectable in all samples, indicating no influence from past nuclear fallout events. The relatively low levels of radionuclides are attributed to the regional geological setting, characterized by alluvial sediments with inherently low radioelement content, as well as processes of weathering, leaching, and quarrying that further reduce radionuclide retention. Radiological hazard parameters were similarly low: the radium equivalent activity ranged from 64 to 97 Bq/kg (mean 80 Bq/kg), well below the recommended limit of 370 Bq/kg; the outdoor and indoor absorbed dose rates (31–48 and 38–57 nGy/h, respectively) were lower than the global average values of 59 and 64 nGy/h; the annual effective doses (0.22–0.34 mSv/y, mean 0.28 mSv/y) remained far below the public dose limit of 1 mSv/y; both the external (0.18–0.27) and internal (0.23–0.33) hazard indices were <1, indicating safe radiological conditions. This study identifies 232Th as the primary contributor to environmental radiological risk, with strong correlations to hazard parameters, while 226Ra and 40K exhibit weaker correlations and distinct geochemical behaviors, highlighting the regional variability of 40K concentrations and the uniformity of 226Ra and 232Th across study sites. Overall, the results demonstrate that quarry pit soils in the studied regions pose negligible radiological risk, providing the first radiological baseline for quarry materials in Bangladesh.