Two hundred and twenty-six breast milk samples were collected from lactating women from 3 blocks of North-24 Paragans, one of the arsenic-affected districts of West Bengal, India. Out of 226 samples, only in 39 samples arsenic was detected. Urine, hair, and nail samples were also analyzed to know the arsenic body burden of the lactating women. Arsenic in drinking water was also analyzed. Principle component analysis (PCA) revealed that hair and nail arsenic was highly correlated with water arsenic concentrations, whereas arsenic in urine and breast milk did not cluster with water arsenic. Our present study indicated that among the lactating women who had high arsenic body burden and arsenical skin lesions, they had elevated level of arsenic in their breast milk. Arsenic in hair, nails, and urine samples of infants were analyzed, and the results showed significantly high-body burden of infants in those areas. PCA showed the age-dependent relationship between the hair and nail arsenic concentrations of the mothers and their babies.