A nanocrystalline PbTiO3 particle/organic hybrid was synthesized through hydrolysis and polymerization of metalorganic compounds below 100 °C. The PbTiO3 precursor was synthesized from lead methacrylate and titanium isopropoxide. The formation of a Pb–Ti complex alkoxide was confirmed by H and Pb nuclear magnetic resonance spectroscopy. Hydrolyzed Pb–Ti alkoxide was polymerized, yielding the PbTiO3 particles/oligomer hybrid. The organic matrix included nano-sized crystalline particles, depending on the hydrolysis conditions. The nanocrystalline particles were identified to be lead titanate by electron diffraction and energy-dispersive x-ray analysis. The dielectric constant of the nanometer-sized PbTiO3/oligomer hybrid was 5.2 at 10 kHz.