Bilayered Pb(Zr(1–x),Tix)O3 ferroelectric thin film heterostructures show complex ferroelastic nanodomain patterns. These ferroelastic nanodomains exist only in the upper layer, and hence are able to move under the application of an external electric field. Quantitative analysis reveals an enhanced piezoelectric coefficient of ≈220 pm V−1, rendering them attractive for a variety of electromechanical devices.