Halide double perovskites have recently bloomed as the green candidates for optoelectronic applications,such as Xray detection. Despite great efforts,the exploration of promising organic-inorganic hybrid double perovskites towardX-ray detection remains unsuccessful. Now,s ingle crystals of the lead-free hybrid double perovskite,( BA) 2 CsAgBiBr 7 (BA + is n-butylammonium), featuring the unique 2D multilayered quantum-confined motif,e nable quite large mt (mobilitylifetime) product up to 1.21 10 À3 cm 2 V À1 .T his figure-ofmerit realized in 2D hybrid double perovskites is unprecedented and comparable with that of CH 3 NH 3 PbI 3 wafers. (BA) 2 CsAgBiBr 7 crystals also exhibit other intriguing attributes for X-rayd etection, including high bulk resistivity,l ow density of defects and traps,a nd large X-raya ttenuation coefficient. Consequently,avertical-structure crystal device under X-rays ource yields as uperior sensitivity of 4.2 mCGy air À1 cm À2 .