Methacrylate zirconium siloxane (MZS) resin was synthesized by a sol-gel reaction of 3-(trimethoxysilyl)propyl methacrylate, diphenylsilanediol, and zirconium n-propoxide chelated with methacrylic acid. Also, propylene glycol monomethyl ether acetate was added as a solvent to synthesize a homogeneous and long-term stable resin by controlling the reactivity among the precursors. A High condensation degree of the resin and the formation of Si-O-Zr hetero-metal bonds were verified by (29)Si NMR and FT-IR spectroscopy. The MZS resin was spin-coated and photo-polymerized to fabricate a highly transparent MZS hybrimer coating film. The refractive index and dielectric constant of the film increased according to the zirconium content, up to 1.59 and 3.65, respectively.