Compositions for golf balls that include organically modified silicates and the golf balls formed using the compositions are described. In particular, the compositions of the invention, which are based on a polyurethane and polysiloxane, polyurea and polysiloxane, and/or epoxy and polysiloxane, and, thus, have the benefits of increased COR, adhesion, and shear and impact resistance. The compositions of the invention may be used in any layer of a golf ball, e.g., an outer cover layer or inner cover layer, or may be used as a coating to be disposed over a structural outer layer of a golf ball.