Chronic exposure to groundwater containing elevated concentrations of geogenic contaminants such as arsenic (As) and uranium (U) can lead to detrimental health impacts. In this study, we have undertaken a groundwater survey of representative sites across all districts of the State of Bihar, in the Middle Gangetic Plain of north-eastern India. The aim is to characterize the inorganic major and trace element aqueous geochemistry in groundwater sources widely used for drinking in Bihar, with a particular focus on the spatial distribution and associated geochemical controls on groundwater As and U. Concentrations of As and U are highly heterogeneous across Bihar, exceeding (provisional) guideline values in~16% and 7% of samples (n = 273), respectively. The strongly inverse correlation between As and U is consistent with the contrasting redox controls on As and U mobility. High As is associated with Fe, Mn, lower Eh and is depth-dependent; in contrast, high U is associated with HCO 3 − , NO 3 − and higher Eh. The improved understanding of the distribution and geochemical controls on As and U in Bihar has important implications on remediation priorities and selection, and may contribute to informing further monitoring and/or representative characterization efforts in Bihar and elsewhere in India.Vaishali, noting importantly that only sources within 10 km of the Ganga River were sampled) [77]. Most recently, it has been reported that 22 districts of Bihar are currently As-impacted, although no further details such as location, non-summarized data or the functional definition of "As-impacted" are included [78]. Further, wheat consumption has recently been identified as an emerging route of As exposure in Bihar [84]. Although thorough reviews of the status of As in the Gangetic Basin are published elsewhere [78,85], the estimated population at risk for As contamination in West Bengal is 26 million people, followed by Bihar (9 million), Uttar Pradesh (3 million), Assam (1.2 million), Manipur (1 million) and Jharkhand (0.4 million) [85]. Widespread in nature, U is a radionuclide which geogenically occurs in granite and other rock types. U in groundwater can occur due to natural mobilization processes under oxic conditions, and can also be associated with anthropogenic activities such as mining, coal and fuel combustion, emissions from the nuclear industry and the use of PO 4 -based fertilizers containing U [4]. As chronic exposure to U may lead to numerous adverse health impacts including bone toxicity and impaired renal function [86,87], WHO has set a provisional guideline value of 0.13 µM (30 µg.L −1 ), noting that Germany adopted a lower threshold of 0.04 µM (10 µg.L −1 ) in 2011 [88]. Elevated concentrations of U in groundwater have been identified across the globe, including in North America (e.g., Canada [89], the United States [90,91]), Europe (e.g., Finland [87], Sweden [92], Switzerland [93], the United Kingdom [94]) and Asia (e.g., Bangladesh [95], China [96,97], Korea [98], Mongolia [99], Pakistan [43] and in the...