The presence of toxic polonium-210 (Po-210) in the environment is due to the decay of primordial uranium-238. Meanwhile, several studies have reported elevated Po-210 radioactivity in the rivers around the world due to both natural and anthropogenic factors. However, the primary source of Po-210 in Langat River, Malaysia might be the natural weathering of granite rock along with mining, agriculture and industrial activities. Hence, this is the first study to determine the Po-210 activity in the drinking water supply chain in the Langat River Basin to simultaneously predict the human health risks of Po-210 ingestion. Therefore, water samples were collected in 2015⁻2016 from the four stages of the water supply chain to analyze by Alpha Spectrometry. Determined Po-210 activity, along with the influence of environmental parameters such as time-series rainfall, flood incidents and water flow data (2005⁻2015), was well within the maximum limit for drinking water quality standard proposed by the Ministry of Health Malaysia and World Health Organization. Moreover, the annual effective dose of Po-210 ingestion via drinking water supply chain indicates an acceptable carcinogenic risk for the populations in the Langat Basin at 95% confidence level; however, the estimated annual effective dose at the basin is higher than in many countries. Although several studies assume the carcinogenic risk of Po-210 ingestion to humans for a long time even at low activity, however, there is no significant causal study which links Po-210 ingestion via drinking water and cancer risk of the human. Since the conventional coagulation method is unable to remove Po-210 entirely from the treated water, introducing a two-layer water filtration system at the basin can be useful to achieve SDG target 6.1 of achieving safe drinking water supplies well before 2030, which might also be significant for other countries.