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This study reports new luminescent oxygen sensors in which the luminophore is covalently bound to the polymer matrix and compares their behavior to related sensors in which the luminophore is dispersed within the matrix. The cyclometalated iridium complex [Ir(ppy)₂(vpy)Cl], 1, has been synthesized and characterized spectroscopically (absorption and emission) and by 1-D and 2-D ¹H NMR, elemental analysis, and X-ray crystallography. Complex 1 was attached via hydrosilation to hydride-terminated poly(dimethylsiloxane) (PDMS), yielding material 2. Successful luminophore attachment was determined spectroscopically from the emission properties, and through the altered physical behavior of 2 compared to a dispersion of 1 in PDMS. Hydrosilation of 1 with dimethylphenylsilane yielded [Ir(ppy)₂(DMPSEpy)Cl], 3, which was fully characterized and used to probe the effect of hydrosilation on the spectroscopic …