This article contains data on the concentration of essential and toxic metals in soils and grains of corn and barley from agricultural areas in the province of Concepción in the Mantaro River Valley, Peru. Analytical determinations of Cu, Fe, Pb, Zn and As were performed by flame atomic absorption spectrophotometry. In corn crop soils, the highest mean concentration of Fe (29,733.72 mg kg−1) was recorded in SC4, Zn (1164.89 mg kg‒1) in SC3, Pb (96.49 mg kg‒1) in SC2, Cu (70.80 mg kg‒1) in SC3 y As (12.66 mg kg‒1) in SC1. In barley soils, the highest mean concentration of Fe (29,400.36 mg kg‒1) was recorded in SB1, Zn (1414.06 mg kg‒1) in SB1, Pb (185.31 mg kg‒1) in SB3, Cu (78.48 mg kg‒1) and As (9.36 mg kg‒1) in SB1. The decreasing order of the highest mean concentration of essential and toxic metals in corn and barley grains was: Fe (207.31 mg kg‒1 in corn and 72.97 mg kg‒1 in barley) > Zinc (45.22 mg g‒1 in corn and 65.58 mg kg‒1 in barley) > Cu (2.21 mg kg‒1 in corn and 19.97 mg kg‒1 in barley) > As (0.100 mg kg‒1 in corn and 0.142 mg kg‒1 in barley). The cluster analysis identified two significantly different groups characterized by the concentrations of heavy metals and arsenic in cultivation soil and cereal grains. The HQ values of Pb and As in corn and barley soils indicated that adverse health effects are unlikely (HQing/derm/inh < 1). Soil HI values of both crops were lower than the permitted value (HI < 1). These data can be reused as a basis for estimating cancer risk from exposure to heavy metals and arsenic in soil and grain of corn and barley or as a comparison group for future risk studies.