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Abstract Mixtures of Ce‐doped rare‐earth aluminum perovskites are drawing a significant amount of attention as potential scintillating devices. However, the synthesis of complex perovskite systems leads to many challenges. Designing the A‐site cations with an equiatomic ratio allows for the stabilization of a single‐crystal phase driven by an entropic regime. This work describes the synthesis of a highly epitaxial thin film of configurationally disordered rare‐earth aluminum perovskite oxide (La_0.2Lu_0.2Y_0.2Gd_0.2Ce_0.2)AlO₃and characterizes the structural and optical properties. The thin films exhibit three equivalent epitaxial domains having an orthorhombic structure resulting from monoclinic distortion of the perovskite cubic cell. An excitation of 286.5 nm from Gd³⁺and energy transfer to Ce³⁺with 405 nm emission are observed, which represents the potential for high‐energy conversion. These experimental results also offer the pathway to tunable optical properties of high‐entropy rare‐earth epitaxial perovskite films for a range of applications.