The　potential　of　forward　osmosis　for　water　treatment　can　only　be　maximized　with　suitable　draw　solutes.　Here　a　three-dimensional,　multicharge　draw　solute　of　decasodium　phytate　(Na10-phytate)　is　designed　and　synthesized　for　removing　organic　arsenicals　from　water　using　a　hybrid　forward　osmosis　(FO)　-　membrane　distillation　(MD)　process.　Efficient　water　recovery　is　achieved　using　Na10-phytate　as　a　draw　solute　with　a　water　flux　of　20.0　LMH　and　negligible　reverse　solute　diffusion　when　1000　ppm　organic　arsenicals　as　the　feed　and　operated　under　ambient　conditions　with　FO　mode.　At　50　°C,　the　novel　draw　solute　increases　water　flux　by　more　than　30%　with　water　fluxes　higher　than　26.0　LMH　on　the　FO　side,　drastically　enhancing　water　recovery　efficiency.　By　combining　the　FO　and　MD　processes　into　a　single　hybrid　process,　a　100%　recovery　of　Na10-phytate　draw　solute　was　achieved.　Crucially,　organic　arsenicals　or　Na10-phytate　draw　solutes　are　both　rejected　100%　and　not　detected　in　the　permeate　of　the　hybrid　process.　The　complete　rejection　of　both　organic　arsenicals　and　draw　solutes　using　hybrid　membrane　processes　is　unprecedented;　creating　a　new　application　for　membrane　separations.　©　2018　American　Chemical　Society.