Accurately characterizing actinide oxides bound to metal–organic frameworks (MOFs) is important for designing MOFs as radioactive waste sorbents and catalytic supports. In this work, the zirconium MOF NU-1000 was post-synthetically modified through solvothermal deposition to include the uranyl (UO₂²⁺) ion and characterized via single-crystal X-ray diffraction. Bond lengths derived from the diffraction pattern and Raman spectroscopy indicate that UO₂²⁺ maintains its chemical properties upon deposition, while alcohol oxidation photocatalysis reveals photo-interactions between the pyrene linkers and the UO₂²⁺ ion.