Food security is a high-priority issue for sustainable global development both quantitatively and qualitatively. In recent decades, adverse effects of unexpected contaminants on crop quality have threatened both food security and human health. Heavy metals and metalloids (e.g., Hg, As, Pb, Cd, and Cr) can disturb human metabolomics, contributing to morbidity and even mortality. Therefore, this review focuses on and describes heavy metal contamination in soil-food crop subsystems with respect to human health risks. It also explores the possible geographical pathways of heavy metals in such subsystems. In-depth discussion is further offered on physiological/molecular translocation mechanisms involved in the uptake of metallic contaminants inside food crops. Finally, management strategies are proposed to regain sustainability in soil-food subsystems.