The luminescent properties of uranyl complexes have been extensively studied; however, fewer investigations have explored their potential applications in ionizing radiation detection. This study delves into the synthesis and structures of a series of uranyl-organic hybrids, as well as their promising use for X-ray scintillation. The combination of uranyl cations with 3-(pyridin-4-yl)benzoate (pba–) organic ligands has yielded a new uranyl-organic hybrid with a 2D network. Notably, U-pba exhibits a distinct radioluminescence, with intensities linearly correlated to X-ray dose rates across a broad dynamic range (36.7–4545.7μGys−1) with a detection limit of 38.12μGys−1. Additionally, it demonstrates high radiation hardness and excellent hydrolytical stability, rendering it as a promising candidate for X-ray scintillation. This work demonstrates that uranyl-organic hybrids represent a promising platform for ionizing radiation detection.