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NaNbO₃(NN)-based lead-free materials are attracting widespread attention due to their environment-friendly and complex phase transitions, which can satisfy the miniaturization and integration for future electronic components. However, NN materials usually have large remanent polarization and obvious hysteresis, which are not conducive to energy storage. In this work, we investigated the effect of introducing CaTiO₃((1−<i>x</i>)NaNbO₃-<i>x</i>CaTiO₃) on the physical properties of NN. The results indicated that as <i>x</i> increased, the surface topography, oxygen vacancy and dielectric loss of the thin films were significantly improved when optimal value was achieved at <i>x</i> = 0.1. Moreover, the 0.9NN-0.1CT thin film shows reversible polarization domain structures and well-established piezoresponse hysteresis loops. These results indicate that our thin films have potential application in future advanced pulsed power electronics.