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Arsenic is a highly toxic metalloid widespread in the Earth's crust, and its contamination due to different anthropogenic activities (application of agrochemicals, mining, waste management) represents an emerging environmental issue. Therefore, different sustainable and effective remediation methods and approaches are needed to prevent and protect humans and other organisms from detrimental arsenic exposure. Among numerous arsenic remediation methods, those supported by using microbes as <i>sorbents</i> (microbial remediation), and/or plants as <i>green factories</i> (phytoremediation) are considered as cost-effective and environmentally-friendly bioremediation. In addition, recent advances in genetic modifications and biotechnology have been used to develop (i) more efficient transgenic microbes and plants that can (hyper)accumulate or detoxify arsenic, and (ii) novel organo-mineral materials for more efficient arsenic remediation. In this review, the most recent insights from arsenic bio-/phytoremediation are presented, and the most relevant physiological and molecular mechanisms involved in arsenic biological routes, which can be useful starting points in the creation of more arsenic-tolerant microbes and plants, as well as their symbiotic associations are discussed.