Remote triggering of smart materials such as shape memory polymers and nanocomposites for drug delivery is a research area of continued interest. Magnetically susceptible nanoparticles (NPs) generate heat when exposed to an alternating magnetic field (AMF), making these NPs an ideal candidate for use in smart nanocomposites. Current research focuses on the impact of surface coating of magnetite NPs on interfacial heat transfer, bulk magnetization properties, and structure of poly(ethylene oxide), PEO, nanocomposites. Bare, poly(ethylene glycol), PEG, coated and amine coated 10–nm–diameter magnetite NPs were dispersed at concentrations less than 1% by weight in PEO. Improved heat generation efficiency was observed for surface modified nanoparticles. The impact of agglomeration and interfacial structure on magnetization and magnetic heating properties was determined through experiments and simulations. This material is based upon work supported by NSF Grant 1825254.