The bulk materials of three-dimensional graphene (3DG) with high network structure and excellent electrical conductivity have many potential applications in flexible electronics, but the network structure is not very stable due to weak bonding between graphene nanosheets. Here, a polyimide (PI) layer was introduced on the as-prepared 3DG sponge by vacuum infiltration–curing method. The resulting 3DG/PI composite sponges with robust 3D network structure exhibited an excellent electrical conductivity (3.7 S/cm), compression strength (175 kPa), elasticity, and flexibility, as well as outstanding compression sensitivity to resistance and stable piezoresistance effect; namely, they possess a large change in resistance in response to application of small strain and low density, and the resistance change remains favorably stable after performing 300 compress–release cycles, which means that the prepared composite sponges can find wide applications in pressure-sensing or stimulus-responsive graphene system.