SummaryAs a finite and non‐renewable resource, phosphorus (P) is essential to all life and crucial for crop growth and food production. The boosted agricultural use and associated loss of P to the aquatic environment are increasing environmental pollution, harming ecosystems, and threatening future global food security. Thus, recovering and reusing P from water bodies is urgently needed to close the P cycle. As a natural, eco‐friendly, and sustainable reclamation strategy, microalgae‐based biological P recovery is considered a promising solution. However, the low P‐accumulation capacity and P‐removal efficiency of algal bioreactors restrict its application. Herein, it is demonstrated that manipulating genes involved in cellular P accumulation and signalling could triple theChlamydomonasP‐storage capacity to ~7% of dry biomass, which is the highest P concentration in plants to date. Furthermore, the engineered algae could recover P from wastewater almost three times faster than the unengineered one, which could be directly used as a P fertilizer. Thus, engineering genes involved in cellular P accumulation and signalling in microalgae could be a promising strategy to enhance P uptake and accumulation, which have the potential to accelerate the application of algae for P recovery from the water body and closing the P cycle.