The present invention is directed to compositions (“Nanomaterial Polymer Compositions”) comprising a silicone polymer and a nanomaterial, including but not limited to, a single or multi-walled nanotube, a nanowire, a nanodot, a quantum dot, a nanorod, a nanocrystal, a nanotetrapod, a nanotripod, a nanobipod, a nanoparticle, a nanosaw, a nanospring, a nanoribbon, a branched nanomaterial, or any combination thereof. The Nanomaterial Polymer Compositions are useful for optical and sensing devices including but not limited to noise suppression, passive Q-switching, mode-locking, waveform shaping, optical switching, optical signal regeneration, phase conjugation or filter devices, dispersion compensation, wavelength conversion, a soliton stabilization, microcavity applications, interferometers; optical, magneto-optical or electro-optical modulation; and biochemical sensors and photodetectors. The Nanomaterial Polymer Compositions are also useful in soft lithography processes.