Few reports are available that characterize daily arsenic exposure through water and diet among people living in groundwater-contaminated regions and correlate it with biomarkers. The present study describes the total individual arsenic exposure and arsenic level in urine and hair of such an arsenic-exposed population in West Bengal. Demographic characteristics and the total daily arsenic intake through water and diet were determined in 167 (Group-1 participants selected from arsenic endemic region) and 69 (Group-2 participants selected from arsenic non-endemic region) in West Bengal. Out of 167 Group-1 participants 78 (Group-1A) had arsenical skin lesions while 89 Group-1B) had no such lesion. Arsenic level in water samples as well as diet, urine and hair samples, collected from all the individual participants, were estimated. The mean value of estimated total arsenic content from water and diet was 349 (range: 20-1615) μg/day in 167 (Group-1) participants living in As endemic region [As in water: mean value 54 (range:BDL-326) μg/L] and 36 (range:12-120) μg/day in 69 (Group-2) participants living in As non-endemic region (As in water: below detection level (BDL), < 0.3 μg/L). Estimated mean arsenic level in urine in these two groups of participants was 116 (range: 6-526) μg/L and 17 (range: BDL-37) μg/L and in hair was 1.0 (range: 0.22-3.98) mg/Kg and 0.16 (range: 0.06-0.37) mg/Kg, respectively. Multiple regressions analysis in Group-1 participants showed that total arsenic intake was associated significantly with urinary and hair arsenic level. The estimated regression coefficient was 0.0022 (95% confidence interval, C.I: 0.0016, 0.0028; P < 0.001) and 0.0024 (95% C.I: 0.0021, 0.003; P < 0.001), respectively. In sub group analysis, higher median urinary arsenic value relative to arsenic intake through water and diet was observed in 78 Group-1A subjects with skin lesion compared to urinary arsenic value in 89 Group-1B subjects without skin lesions, though there was a marginal difference of median total arsenic intake in these two groups. This study showed that significant elevation of arsenic level in urine and hair was associated with elevated arsenic intake through water and diet in people living in arsenic endemic region (Group-1), while these values were low in people living in non-endemic region (Group-2). Those with skin lesions were found to have higher arsenic in urine and hair compared to those without skin lesion with similar arsenic intake through water and diet.