The combination of high atomic number and high oxidation state in UVI materials gives rise to both high X‐ray attenuation efficiency and intense green luminescence originating from ligand‐to‐metal charge transfer. These two features suggest that UVI materials might act as superior X‐ray scintillators, but this postulate has remained substantially untested. Now the first observation of intense X‐ray scintillation in a uranyl–organic framework (SCU‐9) that is observable by the naked eye is reported. Combining the advantage in minimizing the non‐radiative relaxation during the X‐ray excitation process over those of inorganic salts of uranium, SCU‐9 exhibits a very efficient X‐ray to green light luminescence conversion. The luminescence intensity shows an essentially linear correlation with the received X‐ray intensity, and is comparable with that of commercially available CsI:Tl. SCU‐9 possesses an improved X‐ray attenuation efficiency (E>20 keV) as well as enhanced radiation resistance and decreased hygroscopy compared to CsI:Tl. U are scintillating: The observation of intense X‐ray scintillation in a uranyl‐organic framework is reported. Advances are shown in X‐ray attenuation efficiency (E>20 keV) as well as enhanced radiation resistance and decreased hygroscopy when compared to the commercially available scintillator CsI:Tl.