Contamination of soil and water with potentially toxic elements (PTEs) has become a global environmental concern that could pose potential risks to human health and agriculture. The major anthropogenic sources of PTEs contamination include coal combustion processes, leather tanning operations, mining, smelting activities, and use of sewage water for irrigation. Scattered studies are available in the literature that determines the sources, bioavailability, and potential hazards due to PTEs contamination to crop plants and, ultimately, to human beings. This article reviews how solid‐ and solution‐phase chemistry of soil and existing plant species influence the bioavailability of PTEs to cereal and legume plants, along with the mechanisms involved in the uptake and accumulation. This article also describes the phytotoxic effects of PTEs and strategies to overcome these toxic effects by identifying highly tolerant cereals and legumes. Moreover, this article also summarizes recent advances in the field application and discusses perspectives to reduce PTEs accumulation in cereal and legume crops.