Lead‐free perovskite materials have received extensive attention due to their non‐toxicity, super environmental stability and adjustable photoelectric properties. However, the inherent problems of low luminous efficiency and low photoluminescence quantum yields (PLQYs) limit its development in multifunctional applications. Here, Te4+ doped Cs2ZrCl6 with high luminous efficiency and stability for multifunctional applications are developed. Te4+ ions are used as emission centers to improve the optical properties of Cs2ZrCl6 to make efficient and stable single‐component white light‐emitting diodes (WLEDs), and can be used as scintillator materials to improve scintillation performance to achieve high‐resolution and low‐dose X‐ray imaging detection. In addition, it is found for the first time that Te4+ ions can be introduced into the trap center, so that the Cs2ZrCl6:Te4+ perovskite material exhibits excellent persistent luminescence (PersL) and mechanoluminescence (ML) after X‐ray radiation, which has potential applications in the fields of delayed imaging and stress sensing. This work provides a method for designing lead‐free perovskites with high optical performance and scintillating properties, as well as developing multifunctional applications.