This study was conducted to determine concentrations of five toxic trace elements (Cr, Ni, As, Cd, and Pb) in cereals, fruits, and vegetables of Bangladesh. The range of mass fractions (mg/kg) of Cr, Ni, As, Cd, and Pb in the foodstuffs was 0.090–2.5, 0.03–2.6, 0.13–1.7, 0.010–0.74, and 0.37–2.2, respectively. This study indicates that concentration of Cr, and Pb in fruits; As, Cd, and Pb in vegetables were higher than WHO/FAO maximum allowable concentration levels. The hazard index (HI) values for adults and children of the toxic elements in studied cereals, fruits and vegetables were higher than 1.0, suggesting non-carcinogenic adverse health hazard to the consumers. The estimated target carcinogenic risk (TCR) values were greater than the threshold level of 1.0 × 10−4 for Cr and Cd in cereals and vegetables indicate potential cancer risk to both adults and children for consumption of the foodstuffs. The present study reveals that trace elements contamination in foodstuffs is a serious issue of concern in Bangladesh.