Uranium plays an unquestionable role in the framework of nuclear physics, biology, and radiopharmacy. Moreover, uranyl ion UO22+ offers an immense variety of applications due to the unique photosensitivity of its complexes. The excited state of uranyl cation is indeed accessible under ultraviolet‐visible (UV–vis) light, readily producing radical species UO22+* upon light irradiation. Herein, an innovative synthesis protocol is presented to explore the use of uranyl cations as photocatalyst systems for photocurable sol–gel‐based formulations, coupling the photochemical reactions of uranyl cations with photopolymerization‐based additive manufacturing processes. Additive manufacturing has nowadays revolutionized the production of complex structures with arbitrary geometries and has opened up enticing opportunities for innovative technological breakthroughs and highly tailorable systems. The fabrication of micro‐architected components is shown via vat photopolymerization, namely, the Digital Light Processing technique, and ‐3D) printed parts are converted into uranium dicarbide (UC2)/carbon nanocomposite upon carbothermal reduction. This uranyl‐mediated additive manufacturing process constitutes the first application of the synergistic role of uranyl motifs in a photopolymer platform, demonstrating for the first time the possibility to directly pattern uranium‐based materials in complex structures.