Piezoelectric materials perform mechanical-to-electrical energy conversion and have unique and enhanced properties, particularly in the thin film form. In this work, the nanomechanical properties of strontium-doped lead zirconate titanate thin films are investigated by nanoindentation. Finite element modeling of the nanoindentation process allows for a comparison of the simulated and experimentally measured load–displacement curves. New insights correlating the nanomechanical and piezoelectric properties of thin films have been obtained which will enable more efficient design of piezoelectric energy harvesting devices.