Surface modification of aluminum, glass, epoxy resin, polypropylene and polyethylene via corona discharge pretreatment and platinum catalyst addition to promote their adhesion with liquid silicone rubber is reported. The corona-pretreated substrate surface was silanized with vinyltrimethoxysilane to generate vinyl groups on the surface, which could be initiated by platinum catalyst to form vinyl radicals. Then, the vinyltrimethoxysilane modified substrate was dipped into platinum catalyst solution to introduce platinum on the vinyltrimethoxysilane surface. The modified aluminum surface was characterized by X-ray photoelectron spectroscopy (XPS). The strong adhesion property between liquid silicone rubber and different surface was achieved by introducing a small amount of vinyltrimethoxysilane and platinum catalyst, followed by curing at low temperature. XPS result indicated the formation of vinyltrimethoxysilane coating on aluminum surface. Peel strength for liquid silicone rubber/vinyltrimethoxysilane–platinum surface was over 3·2 kN/m compared to only 1·1 kN/m for liquid silicone rubber/vinyltrimethoxysilane–aluminum. The cohesive failure in the bulk of liquid silicone rubber was observed for liquid silicone rubber/vinyltrimethoxysilane–platinum surface. It is assumed that the cross-linking reactions between vinyl groups in the vinyltrimethoxysilane coating and unsaturated terminal group of liquid silicone rubber occur due to the existence of platinum catalyst.