The reported work highlights that both polarizibility and quasi-DC conductivity, the two most important parameters for high energy density materials, can be influenced by the surface polarity of an oxide and interfacial surface tension between the oxide and polymer in a laminar composite. Surface modification of laminar composites, composed of thermally grown silica and vapor phase grown Parylene C thin films using organosilanes, was used to control silica surface polarity and interfacial surface tension. Surface polarity of thermally grown silica was found to control the interfacial dipolar energy states.