Interface interaction between filler and rubber molecules is a key to the properties of the composites. In this research, we aimed to improve the interface between graphene (GE) and chloroprene rubber (CR). Therefore, ZnO-GE hybrids were prepared by thermal treatment of the mixture of Zn(OH)2 and graphene oxide at high temperature. The ZnO nanoparticles were uniformly coated on the surface of the GE. The ZnO-GE hybrids were further compound with chloroprene rubber (CR). During the curing process, ZnO attached by GE can have a crosslinking reaction with CR molecules. Finally. GE was firmly attached with CR molecules by the ionic bond between ZnO and CR. The results showed the ZnO-GE particles was dispersed well in the CR. The ZnO-GE/CR composites had improved mechanical properties, abrasion property and high electrical property, due to the strong interface interaction.