Combining computations and X-ray structure analysis we have demonstrated that [Pt(CN4)]2- can behave as a Lewis acid inside an enzyme's cavity. The nature of a counterintuitive contact found between a catalytically active GLN residue belonging to a mitochondrial synthase and the Pt(II) center was investigated by combining molecular dynamics and quantum mechanics calculations. Results confirm the electron acceptor role of [Pt(CN4)]2-, serving as an inspiration for the design of biomolecular cages able to tweak the nucleophilic/electrophilic character of an organometallic compound.