This study presents a multi‐mode X‐ray detection and imaging strategy by integrating photochromism, photoluminescence, and radioluminescence into Tb3+‐doped CaAl2Si2O8. CaAl2Si2O8: Tb3+ exhibits stable radioluminescence, oxygen vacancy‐related photochromism, and photoluminescence modulation, all of which showed a linear relationship with X‐ray exposure. This multi‐mode response enables high‐quality imaging and detection in both bright and dark conditions, facilitating time‐dependent cumulative X‐ray radiation dose assessments. Reversible color and luminescence changes are achieved through cyclic tests involving alternating X‐ray and 473 nm laser irradiation. The PDMS CaAl2Si2O8: Tb3+ ink and flexible film demonstrate high suitability for wearable X‐ray detection devices and imaging of irregular objects, offering an innovative approach to X‐ray detection and imaging.