AbstractTo improve the interfacial bonding between hollow microspheres (RiM01) and natural rubber (NR), the silane coupling agents γ‐aminopropyltriethoxysilane (KH550) and γ‐methacryloyloxypropyltrimethoxysilane (KH570) are used in this study as intermediate reaction platforms for the modification of (RiM01) with glycidyl methacrylate (GMA), respectively. In the process, GMA reacts with KH550 and KH570 through epoxy group ring‐opening and free radical polymerization, respectively. Different NR/RiM01@GMA composites are prepared by a mechanical blending method. The results show that the addition of GMA improves the interfacial bonding between RiM01 and NR, and enhances the vulcanization rate and cross‐linking degree of the rubber composites. When KH550 is used as the reaction platform, the tensile strength of the rubber composites increases by 24% compared to composites with unmodified RiM01, while when KH570 is used, the tensile strength increases by 18%. Additionally, the tear strength and abrasion resistance of the rubber composites increase by 13% and 15%, respectively, when KH570 is used as the reaction platform. At the same time, the filler‐matrix interaction is strongest when KH570 is used as the reaction platform, and the rubber composites exhibit the lowest rolling resistance and the best resistance to heat and oxygen aging.Highlight Modification of hollow microspheres by grafting GMA with KH550 and KH570, respectively. Improvement of rubber composite properties after modification GMA improves the interfacial bonding between hollow microspheres and rubber.