The health effects of drinking water exposure to inorganic arsenic are well known but are less well defined for dietary exposure. The rising concerns of arsenic risks from diet motivated this study of arsenic concentrations in highland barley, vegetables, meat, and dairy products to evaluate arsenic exposure source and to assess health risks among rural residents of Ngari area, western Tibet. Total arsenic and arsenic speciation were measured by inductively coupled plasma mass spectrometry (ICP-MS) and high-performance liquid chromatography combined with ICP-MS (HPLC-ICP-MS) respectively. Average total arsenic concentrations of 0.18 ± 0.21 (n = 45, median: 0.07 mg·kg？1), 0.40 ± 0.57 (n = 17, median: 0.15 mg·kg？1), 0.21 ± 0.16 (n = 12, median: 0.17 mg·kg？1), and 0.18 ± 0.08 (n = 11, median: 0.22 mg·kg？1) were observed in highland barley, vegetables, meat, and dairy products, respectively. Inorganic arsenic was determined to be the main species of arsenic in highland barley, accounting for about 64.4 to 99.3% (average 83.3%) of total arsenic. Nearly half (44.4%) of the local residents had ingested >3.0 × 10？4 mg·kg？1·d？1 daily dose of arsenic from highland barley alone, above the maximum oral reference dose recommended by the United States Environmental Protection Agency (USEPA). The inorganic arsenic daily intake from highland barley was 3.6 × 10？4 mg·kg？1·d？1. Dietary exposure to inorganic arsenic alone increased the cancer risk probability to 5.4 in 10,000, assuming that the inorganic arsenic in highland barley has the same carcinogenic effects as that in water.