The ¹³⁷Cs and ⁴⁰K activities and transfer factors from soil to vegetables, grass, and milk from villages located around Tarapur Atomic Power Station (TAPS) were determined using high-resolution gamma spectrometry. A total of 32 soil, 21 vegetable, 23 dry paddy grass, and 23 milk samples were collected from 23 different agricultural farms from various villages around TAPS to determine transfer factors for natural environment. The mean concentration values for ¹³⁷Cs and ⁴⁰K in soil, grass, and milk were 2.39±0.86 Bq kg⁻¹, 0.31±0.23 Bq kg⁻¹, and 12.4±5.7 mBq L⁻¹ and 179±31 Bq kg^{− 1}, 412±138 Bq kg^−1, and 37.6±9.3 Bq L⁻¹, respectively, for soil–grass–milk pathway. In the soil–vegetation pathway,the mean concentrations values for ¹³⁷Cs and ⁴⁰K were 2.15±1.04 Bq kg^−1, 16.5±7.5 mBq kg⁻¹,and 185±24, 89±50 Bq kg⁻¹, respectively. The evaluated mean transfer factors from soil–grass, grass–milk, and soil vegetation for ¹³⁷Cs were 0.14,0.0044, and 0.0073 and that of ⁴⁰K were 2.42, 0.0053,and 0.49, respectively. Only 15 out of total 44 milk and vegetable samples were detected positive for ¹³⁷Cs, indicating a very low level of bioavailability.