Ethylene-methacrylic acid ionomer (Surlyn) with concentration up to 20 wt% based on total weight of polymer resin was added into polypropylene (PP)/organoclay hybrids. The microstructure, rheological properties, crystallization properties and mechanical properties of the obtained nanocomposites have been investigated. The addition of ionomer markedly enlarged interlayer spacing of the platelets and led to an improved degree of exfoliation. Moreover, clay silicates were found to selectively disperse either inside the ionomer phase or at the phase boundary. Compared to the binary immiscible blends, an improved interfacial adhesion was achieved for PP/Surlyn/OMMT hybrids. Unlike PP/Surlyn binary blends, the viscoelastic properties of the hybrids significantly increased with increasing Surlyn concentration, which could be attributed to the improved clay dispersion and the contribution of silicate layers at the interface between PP and Surlyn. A synergistic role between Surlyn and clay was also found to suppress the crystallization of PP matrix. In addition, PP/Surlyn/OMMT hybrids exhibited superior tensile strain compared to the corresponding PP/PP-g-MA/OMMT. Both tensile strength and elongation at break showed maximum at Surlyn concentration of 5 wt%. By comparing the experimental tensile yield strength with model prediction, it was suggested that the clay platelets localized at the interface could play a role of interfacial activation to some extent.