These flat-panel X-ray detectors present high sensitivity and low detection limit, but suffer from high cost, complex configuration, and are not applicable to directly image irregular objects. [3] Accordingly, it is urgent to develop largearea, flexible structure with simple configuration, low cost, and high sensitivity detectors for advanced X-ray imaging. Among them, flexible detectors consisting of X-ray storage materials are emerging as one of promising candidates owing to their simple configuration, convenient readout processes, and abilities to enable X-ray imaging in less accessible situations. [3b,4] X-ray storage phosphors show X-rayactivated persistent luminescence (X-PersL) that can store excitation energy and give a sustained release of photon emissions with a duration of few seconds to days. [5] X-PersL materials (e.g., BaFCl:Eu 2+ ) were first used in imaging plates for commercial computed radiography (CR) by Fujifilm in 1983. [6] However, the development of these materials for X-ray imaging has made very little progress since then. [7] Recently, Ou et al. renovated the existing X-ray imaging technology via embedding X-PersL nanoparticles into silicone polymer as a flexible and stretchable detector. [3b] Their photophysical characteristics of excitation and emission separation allow time-lapse and convenient imaging, enabling simplification of the X-ray imaging system and visualization of X-ray imaging free from dangerous radiation. [4] Generally, X-ray storage materials should have excellent X-ray absorption capacity, low-temperature formation of crystalline, and energy traps with controllable properties. Defects play the crucial role in regulation of trap properties, which determine the storage capacities for X-ray imaging. [4,8] In the past few decades, researchers have made great efforts to develop inorganic oxidebased storage phosphors. Nevertheless, low X-ray sensitivity and high synthetic temperature as well as harsh conditions for generating appropriate energy traps limit their further applications. By contrast, halide perovskites are emerging as next-generation optoelectronic materials in recent years, which have the advantages of X-ray sensitivity, processable at low temperature, low-cost, and superior photophysical properties. [9] Despite some metal halide perovskite compounds show PersL, such as Cs 2 AgInCl 6 :Mn 2+ , [10] Cs 3 In 2 Cl 9 , [11] it remains a challenge to realize 3D X-ray imaging by using these materials due to their low storage capacities.In this work, we report the rational design and controlled synthesis of X-ray storage phosphor CsCdCl 3 :xMn 2+ , yR 4+ X-ray imaging has received sustained attention for healthcare diagnostics and nondestructive inspection. To develop photonic materials with tunable photophysical properties in principle accelerates radiation detection technologies. Here the rational design and synthesis of doped halide perovskite CsCdCl 3 :Mn 2+ , R 4+ (R = Ti, Zr, Hf, and Sn) are reported as next generation X-ray storage phosphors, and the capa...