Recycling the arsenic-rich biomass of Pteris vittata is a critical problem during phytoremediation primarily because of the low value and high risk of arsenic-rich biomass. Nevertheless, extracts of P. vittata have been found to have a variety of bio-activities (e.g., anti-oxidation, anti-cancer, and anti-bacterial) and abundant valuable bio-active compositions (e.g., flavonoids), which might present a new solution for the recycling of P. vittata harvests. This work demonstrated a pilot-scale experiment to extract and purify the phenolic compounds from 1 t of arsenic-rich P. vittata biomass. Result showed that 47.9 kg of phenolic-rich extract with a potential value of US$908.66-8345.14 was obtained. This extract showed no acute oral toxicities (LD50 > 10 g/kg), no skin irritation, and no chronic risks in the long-term skin contact exposure pathways. All of the wastes from production have been recycled and safely disposed with low cost (US$28.44), and the cost may be further reduced. The calculated benefits from this method showed a potential to provide 995-53,050 US$/hm2 per year to a phytoremediation project. Therefore, this strategy could address the issue of expensive phytoremediation.