This study investigated the contamination levels and sources of As and Cd vicinity area from Nui Phao mine that is one of the largest tungsten (W) open pit mines in the world. Soil and plant samples were collected from the study area to identify the concentrations of As and Cd using aqua-regia or HNO3 digestion. According to the Vietnamese agricultural soil criteria, all soil samples were contaminated with As and Cd. The distribution of As concentration is related to the distance from the Nui Phao mine. The higher As concentrations were measured in the area close to the mine. However, the Cd distribution in the soil showed a different pattern from As. Enrichment factor and Geoaccumulation Index (Igeo) indicated that As in the soil is derived from the mining activities, while Cd could have other geogenic or anthropogenic sources. The ranges of As and Cd concentration in polished rice grains in the Nui Phao mine area exceeded the CODEX criteria (0.2 mg/kg), which indicated extreme contamination. The arsenic concentration between soil and plant samples was determined to be a positive correlation, while the Cd concentration showed a negative correlation, implying that As and Cd have different geochemical behavior based on their sources.