Cu-functionalized UiO-67 MOFs were prepared as heterogenized homogeneous catalysts. Operando XAS, FTIR and DFT shed light on Cu-species in catalysis-relevant states. Well-defined redox-active Cu-complexes are found at specific location in the MOF. Cu-carbonyl interaction in Cu-UiO-67 MOFs was identified and described. Future operando studies will explore redox catalysis on these promising Cu-sites.