Metalloids are a subset of particular concern to risk assessors and toxicologists because of their well-documented potential hazards to plant system. Most of the metalloids are major environmental contaminants which affect crop productivity when present in high concentrations in soil. Metalloids are coupled with carrier proteins of the plasma membrane and translocated to various organs causing changes in key metabolic processes, damages cell biomolecules, and finally inhibit its growth. Phytoremediation-based approaches help in understanding the molecular and biochemical mechanisms for prerequisite recombinant genetic approaches. Recent advancements in proteomics and plant genomics help in understanding the role of transcription factors, metabolites, and genes in plant system which confers metal tolerance. The present review summarizes our current status of knowledge in this direction related to various physiological responses, detoxification mechanisms, and remediation strategies of metalloids in crop plants in relation to plant-metalloid tolerance. Further, the role of various transcription factors and miRNAs in conferring metal tolerance is also briefed. Hence, the present review mainly focused on the alterations in the physiological activities of plants due to metalloid toxicity and the various mechanisms which get activated inside the plants to mitigate their toxic effects.