Thermoresponsive magnetic nanoparticles (MNPs) as a class of smart materials that respond to a change in temperature may by used as a draw solute to extract water from brackish or seawater by forward osmosis (FO). A distinct advantage is the efficient regeneration of the draw solute and the recovery of water via heat-facilitated magnetic separation. However, the osmotic pressure attained by this type of draw solution is too low to counteract that of seawater. In this work, we have designed a FO draw solution based on multifunctional Fe3O4 nanoparticles grafted with copolymer poly(sodium styrene-4-sulfonate)-co-poly(N-isopropylacrylamide) (PSSS-PNIPAM). The resulting regenerable draw solution shows high osmotic pressure for seawater desalination. This is enabled by three essential functional components integrated within the nanostructure: (i) a Fe3O4 core that allows magnetic separation of the nanoparticles from the solvent, (ii) a thermoresponsive polymer, PNIPAM, that enables reversible clustering of the particles for further improved magnetic capturing at a temperature above its low critical solution temperature (LCST), and (iii) a polyelectrolyte, PSSS, that provides an osmotic pressure that is well above that of seawater.