Example embodiments of the present invention relate to an organic-inorganic hybrid polymer having capped terminal hydroxyl groups and an organic insulator composition including the hybrid polymer and methods thereof. The organic-inorganic hybrid polymer may be prepared by capping terminal hydroxyl groups of silanol moieties that do not participate in the formation of an intermolecular network in an organic-inorganic hybrid material, with an organosilane compound. The organic-inorganic hybrid polymer may increase the hysteresis and physical properties of an organic thin film transistor. The organic-inorganic hybrid polymer may be more effectively utilized in the manufacture of liquid crystal displays (LCDs).