The purpose of this study was to identify the concentration of multi-elements (MEs) in source water (surface and drinking water) and assess their quality for sustainability. A total of 161 water samples including 88 tap drinking waters (DW) and 73 surface waters (SW) were collected from five cities in Xi’an, Yan’an, Xining, Lanzhou, and Urumqi in northwestern China. Eighteen parameters including pH, electrical conductivity (EC), total organic carbon (TOC) total nitrogen (TN), chemical compositions of anions (F−, Cl−, NO3−, HCO3−, SO42−), cations (NH4+, K+, Na+, Ca2+, Mg2+), and metals (lead (Pb), chromium (Cr), cadmium (Cd), copper (Cu)) were analyzed in the first time at the five cities . The results showed that pH values and concentrations of Cl−, SO42−, Na+, K+, Ca2+, Mg2+ and Cd, Cr, Cu in DW were within the permissible limits of the Chinese Drinking Water Quality Criteria, whereas the concentrations of other ions (F−, NO3−, NH4+ and Pb) exceeded their permissible values. In terms of the SW, the concentrations of F−, Cl−, NO3−, SO42− were over the third range threshold i.e., water suitable for fishing and swimming of the Surface Water Quality Standards in China. The spatial distributions of most MEs in source water are similar, and there was no clear variation for all ions and metals. The metals in DW may be caused by water pipes, faucets and their fittings. The noncarcinogenic risk of metals in DW for local children are in decreasing order Cr > Cd > Pb > Cu. The carcinogenic risk from Cr exposure was at the acceptable level according to threshold of USEPA. Although the comprehensive index of potential ecological assessment of Cr, Cd, Pb and Cu in SW ranked at low risk level and was in the order of Huang River in Xining > Peaceful Canal in Urumqi > Yan River in Yan’an > Yellow River in Lanzhou, their adverse effects to ecology and human health at a low concentration in local semi-arid and arid areas should not be ignored in the long run.