PZT films were deposited by the sol-gel method on platinized silicon substrates with silicon nitride and silicon oxide structural layer materials. The crystalline orientations of the PZT films were controlled by both a chelating agent and pyrolysis temperature. A nanoindentation CSM (continuous stiffness measurement) technique was utilized to characterize the Young's moduli of these PZT films. It was found that the measured moduli of PZT films on the two types of substrates showed similar orientation dependence (E-001 > E-111> E-(110,E-111)) but distinct values, which indicated a clear substrate effect. By using a new model of film indentation, we were able to decouple the effects of film orientation and structural layer type on the Young's modulus.