Forward　osmosis　(FO)　has　been　increasingly　used　for　water　treatment.　However,　the　lack　of　suitable　draw　solutes　impedes　its　further　development.　Herein,　we　design　pH-responsive　polyoxometalates,　that　is,　(NH4)6Mo7O24and　Na6Mo7O24,　as　draw　solutes　for　simultaneous　water　reclamation　and　resource　recovery　from　wastewater　via　FO.　Both　polyoxometalates　have　a　cage-like　configuration　and　release　multiple　ionic　species　in　water.　These　characteristics　allow　them　to　generate　high　osmotic　pressures　to　drive　the　FO　separation　efficiently　with　negligible　reverse　solute　diffusion.　(NH4)6Mo7O24and　Na6Mo7O24at　a　dilute　concentration　(0.4　M)　produce　water　fluxes　of　16.4　LMH　and　14.2　LMH,　respectively,　against　DI　water,　outperforming　the　frequently　used　commercial　NaCl　and　NH4HCO3draw　solutes,　and　other　synthetic　materials.　With　an　average　water　flux　of　10.0　LMH,　(NH4)6Mo7O24reclaims　water　from　the　simulated　glutathione-containing　wastewater　more　efficiently　than　Na6Mo7O24(9.1　LMH),　NaCl　(3.3　LMH),　and　NH4HCO3(5.6　LMH).　The　final　glutathione　treated　with　(NH4)6Mo7O24and　Na6Mo7O24remains　intact　but　that　treated　with　NaCl　and　NH4HCO3is　either　denatured　or　contaminated　owing　to　their　severe　leakage　in　FO.　Remarkably,　both　polyoxometalates　are　readily　recycled　by　pH　regulation　and　reused　for　FO.　Polyoxometalate　is　thus　proven　to　be　an　appropriate　candidate　for　FO　separation　in　wastewater　reclamation　and　resource　recovery.　©　2021　American　Chemical　Society