In order to mitigate nutrient pollution in surface runoff more sustainably, the finite capacity for phosphorus (P) sequestration in best management practices (BMP) that rely heavily on sorption processes must be addressed. These BMP include sand filters, bioretention cells, and several types of constructed wetland. This study investigated facilitated microbial reduction of iron-based filtration substrates to promote controlled release of P previously sequestered by the BMP, P harvest for recycling, and rejuvenation of the substrate sorption capacity. Total dissolved P was well correlated with total dissolved iron during the reduction process, indicating that microbial iron reduction was capable of releasing previously sequestered P from substrates. Furthermore, results indicated that a sufficient carbon source was necessary but addition of a microbial culture was not necessary to facilitate iron reduction. While a large percentage of the previously sequestered P was removed, the process was much slower than initial sequestration of P by adsorption, and further research is needed to promote a more rapid release of P in order to optimize the rejuvenation process for field application.