Achieving specific interactions of metal-oxo clusters with biological substrates becomes possible through organic functionalization. The illustration depicts a dartboard that symbolizes the enzyme's active site as the molecular target. The darts represent clusters bearing distinct organic functionalities, designed to enable selective interactions with the protein surface. This concept highlights the potential of molecular design strategies to achieve precise bioinorganic recognition. More in the Communication (e202518349) by Mhamad Aly Moussawi, Tatjana N. Parac-Vogt, and co-workers.