The Eu‐doped compositionally graded multilayer PbZrO3 antiferroelectric thin films have been deposited on Pt(111)/Ti/SiO2/Si
substrates by a sol–gel method. The effect of gradient sequence on microstructure, electrical properties, and energy storage performance has been investigated in detail. X‐ray
diffraction patterns confirm that both thin films have crystallized into a unique perovskite phase. Down‐graded thin films have bigger grain sizes than up‐graded films, which is attributed to the influence of the gradient sequence of the thin films layer. The dielectric constant
of down‐graded films is found to be higher than that of up‐graded films. Compared with up‐graded thin films, the energy storage density of down‐graded films is enhanced due to double hysteresis loop with small hysteresis switch, and high polarization.