Within the microelectronics industry, there is an ongoing trend toward miniaturization coupled with higher performance. High glass-transition temperature polynorbornenes exhibit many of the key performance criteria necessary for these demanding applications. However, homopolynorbornene exhibits poor adhesion to common substrate materials, including silicon, silicon dioxide, aluminum, gold, and copper. In addition, this homopolymer is extremely brittle, yielding less than 1% elongation-to-break values. To address these issues, the homopolymer was functionalized to improve adhesive and mechanical properties. Attacking triethoxysilyl groups to the polymer backbone substantially improved the adhesion, but at the cost of increasing the dielectric constant because of the polarity of the functional group. Alkyl groups were also added to the backbone, which decreased the rigidity of the system, and resulted in significantly higher elongation-to-break values and a decrease in residual stress. The addition of an alkyl group slightly decreased the dielectric constant of the polymer as a result of an increase in molar volume. The coefficient of thermal expansion and modulus are also reported for the polynorbornene functionalized with triethoxysilyl groups using a multiple substrate approach.