This research aims to assess the content of some ions and trace elements in water sources in 24 rural Roma communities in Transylvania in order to assess the human health risk associated with exposure to such elements and ions. To this end, eight ions (F−, Cl−, Br−, NO2−, NO3−, SO42−, PO43−, NH4+) and ten trace elements (Cr, Ni, As, Pb, Cd, Mn, Cu, Zn, Fe, and Hg) were determined in 71 water samples by ion chromatography coupled with a conductivity detector for ions and atomic absorption spectrophotometry for all trace elements. General parameters were also determined. Non-conformity (as number of samples), according to the EU Drinking Water Directive, was observed as follows: pH (7), EC (7), hardness (1), oxidizability (15), Cl− (4), NO3− (30), SO42− (6), Fe (16), Mn (14), As (3), and Ni (1 sample). The incidence of ions was Cl− (71), SO42− (70), F− (67), NO3− (65), NH4+ (21), Br− (10), PO43−, and NO2− (1 sample) and for trace elements, Mn (59), Fe (50), As (38), Ni (32), Cu (29), Zn (28), Cd (12), Cr (11), and Pb (3 samples). Hg was not detected. Non-carcinogenic (HI) values exceeded one for As in 13 Roma communities, with higher values for children than for adults. For NO3−, the HI values were >1 in 12 for adults and 14 communities for children. The carcinogenic risk (CR) for As through ingestion ranged from 0.795 to 3.50 × 10−4 for adults and from 1.215 to 5.30 × 10−4 for children. CR by dermal contact was in the range of ×10−6 both for adults and children.