Novel multifunctional core-shell nanoparticles (Fe3O4@PSBMA NPs) with magnetic and zwitterionic properties were first synthesized and efficiently incorporated into the poly(vinylidene fluoride) (PVDF) membranes via magnetically controlled surface segregation toward the better water-energy-food nexus. The combination of zwitterionic polymers poly(sulfobetaine methacrylate) (PSBMA) and Fe3O4 particles can improve the compatibility of additives with the PVDF matrix and significantly improve the migration of Fe3O4@PSBMA NPs onto membrane surfaces under magnetic fields during nonsolvent-induced phase separations. The modified membrane with surface-enriched multifunctional zwitterionic NPs had an enhanced water flux (168%, ∼630.5 L m-2 h-1), excellent fouling resistance (∼93.8%), and increased rejection to bovine serum albumin (94.1%). Most importantly, the PVDF/M-Fe3O4@PSBMA membrane had excellent stability under the long-term filtration test for practical water-treatment applications.