Arsenic (As) contamination in soil poses a serious threat to ecosystem and human health. Different physical and chemical methods are employed to mitigate this problem, but they have several inherent drawbacks including high cost, energy intensive and eco-invasive nature. Whereas phytoremediation is an eco-friendly, cost-effective and sustainable strategy for remediation of soil As contamination. Pteridophytes have evolutionary advantages that allow them to accumulate contaminants from soil, thus acting as natural scavenger of soil contaminants. Chinese brake fern (Pteris vittata L.) is credited with the distinction of being ‘first’ arsenic hyperaccumulator exhibiting remarkable potential for arsenic removal from contaminated soils up to 22,630 mg kg-1 As in its dry mass. In this review starting with a brief outline of the taxonomy of phytoremediation, the molecular mechanisms of accumulation, translocation, and detoxification of As in pteridophytes have been highlighted with special reference to P. vittata. Further, the means and measures of maneuvering phytoremediation have been discussed with an objective of enhancement of its performance and success in environmental remediation.