This paper reports on the use of poly(dimethylsiloxane) (PDMS) thin films to bond pairs of glass slides, borosilicate glass, and silicon substrates, with an emphasis on application for wafer-level three-dimensional (3D) heterogeneous integration technology platforms. PDMS films were spin-cast and cured, surface modified using low power oxygen plasma, and then bonded to various materials. These bonds were destructively tested using a four point bending technique. The critical adhesion energy obtained using surface modified PDMS to bond glass slides is 3.0 J/m2. Adhesion energies obtained using unmodified PDMS are 2.8, 1.8, and 1.6 J/m2 for bonded silicon, glass slides, and borosilicate glass, respectively. Correlation of these results to material surface and interface properties indicates that although PDMS has process advantages as a bonding material for heterogeneous integration, its adhesion strength is lower than that of other dielectric bonding glues.