The ability to form blends of polymers offers the opportunity of creating a new class of materials with enhanced properties. In addition to the polymer components, recent advances in nanoengineering have resulted in the development of nanosized inorganic particles that can be used to improve the properties of the blend, such as the flammability and the mechanical properties. While traditional methods using copolymer compatibilizers have been used to strengthen polymer blends, here, we show that the inorganic nanosized filler additive can also serve as a compatibilizer as it can localize to the interface between the polymers. We use experimental and theoretical studies to show the fundamental mechanisms by which inorganic fillers with large aspect ratio and at least one-dimension in the nanometer range, can act as non-specific compatibilizers for polymer blends. We examine a series of nanosized fillers, ranging from nanotubes to nanoclays (with varying aspect ratios) in a model polystyrene (PS)/poly(methylmethacyralate) (PMMA) blend. Using a number of experimental techniques such as transmission electron microscopy (TEM), scanning tunneling X-ray microscopy (STXM), and atomic force microscopy (AFM) we postulate that the mechanism of compatibilization occurs as a result of the fillers forming in situ grafts with the immiscible polymers. We also use theoretical studies to show that the aspect ratio and the bending energy of the fillers play a key role in the compatibilization process. Our results indicate that the compatibilization is a general phenomenon, which should occur with all large aspect ratio nanofiller additives to polymer blends.Studies have also demonstrated how colloidal particles are interfacially active agents. [9] Several groups have demonstrated that when nanoscale fillers are added to phase-segregating (wileyonlinelibrary.com)