application necessitating specific detection and efficient shielding of X-ray. [1] In general, radiation detection and radiation shielding are cataloged as two different disciplines. [2] The former focused on directly or indirectly converting invisible ionizing radiation into readable signals by ionization chambers, semiconductor detectors, scintillation counters, and so on. [3] For the latter field, high mass elements (Z) including Pb, W, and Bi, etc., are utilized to attenuate X-ray radiation, since the shielding efficacy is dependent on Z-value and density of the absorbing materials. [4] The bonding between these two areas appears to be weak at first glance. However, high Z-value elements are often preferred as well for building X-ray scintillators and semiconductor detectors, which renders constructing a dual-module platform of radiation detection and shielding plausible. [5] However, developing this type of proof-of-concept materials has not been documented and a single material integrating both functions remained elusive.Radiochromic organic-inorganic hybrids represent a relatively new type of material with the potential to be a dualmodule platform for radiation detection and shielding. [6] As one of the most sensible detection technologies, radiochromic materials turn colors upon being irradiated, which allows for straightforward detection of X-ray radiation in a visible manner. [7] Furthermore, the fine control over the metal cations and organic ligands in organic-inorganic hybrids offers a large set of synthetically accessible combinations in terms of composition and arrangement, an attribute that is absent in purely inorganic or organic materials. [8] Indeed, scintillating and semiconductive organic-inorganic hybrids with high X-ray sensitivity have emerged as new classes of radiation detectors. [9] Moreover, radiochromism has been realized in organic-inorganic hybrids by incorporating photochromic ligands and metal cations or clusters. [6,10] However, only a handful of these types of materials have been reported and their attenuation efficiencies of ionizing radiation remain underexplored. [6,10a,11] Our group has been recently focused on developing new synthetic strategies to access thorium-based crystalline materials for their promising applications in radiological fields. [12] As the second heaviest naturally occurring element, thorium can serve Monitoring and shielding of X-ray radiation are of paramount importance across diverse fields. However, they are frequently realized in separate protocols and a single material integrating both functions remained elusive. Herein, a hexanuclear cluster [Th 6 (µ 3 -OH) 4 (µ 3 -O) 4 (H 2 O) 6 ](pba) 6 (HCOO) 6 (Th-pba-0D) incorporating high-Z thorium cations and 3-(pyridin-4-yl)benzoate ligands that can function as a brand-new dual-module platform for visible detection and efficient shielding of ionizing radiation is demonstrated. Th-pba-0D exhibits rather unique reversible radiochromism upon alternating X-ray and UV irradiation. Moreover, the millimet...