Display omitted •Simultaneously evaluated the contamination of F− and arsenic in surface water.•Total and bio-available F− and arsenic in soil.•F− and arsenic contents in grain crops and their bio-concentration factor.•Estimated daily intake and risk assessment of F− and arsenic in different age groups. The aim of present study was to simultaneously estimate the arsenic (As) and fluoride (F−) concentrations in irrigated surface water, soil and grain crops of Nagarparkar, Pakistan during 2010–2012. The As and F− were analyzed by hydride generation atomic absorption spectrometer and ion selective electrode, respectively. Total arsenic (AsT) and F− in irrigated surface water samples were found in the range of 360–683μgL−1 and 18.5–35.4mgL−1, respectively. While AsT and F− concentrations in agriculture soil samples were observed in the range of 110–266 and 125–566mgkg−1, respectively. The water extractable As and F− were found 3–4% of total concentration of these in soils. The AsT concentration was higher in kidney been (KB) as compared to pearl millet (PM) and green gram (GG), whereas GG had higher F− levels as compared to other two grain crops (p<0.05). The KB samples grown in nine sites shows BCF of As in the range of 0.018–0.038. The GG has higher BCF of F− as compared to KB and PM (p<0.05) grown in all sites. The exposure dose and risk factor of As and F− were obtained by estimated daily intake (EDI) and hazardous index (HI). It was found that all understudy age groups were at the severe risk of arsenicosis and fluorosis, but the severity is higher in younger age group (7–15years) as compared to elder groups (p<0.05).