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Dielectric nanomaterials offer great promise for diverse technological applications such as capacitors, actuators, and sensors. Unfortunately, the exploitation of desirable dielectric properties in polymer nanocomposites is a great challenge due to lack of efficient routes to achieve uniform dispersion of nanoparticles and good compatibility of interfaces at high nanoparticle loadings. A dilemma between the nanofiller loading and dispersion as well as interfacial compatibility makes it impossible to fully exploit the intrinsic polarization of the nanoparticles. Herein, we solve such a dilemma and fabricate highly filled barium titanate/silicone rubber (BT/SR) nanocomposites through chemically bonding BT nanoparticles with SR by “thiol–ene click” and isostatic pressing techniques. BT loading varies from 88 wt% to 97 wt% without compromising the uniform dispersion quality and good interfacial adhesion with the SR matrix …