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However, the balance between their Lewis acidic and basic functions is normally fixed by molecular synthesis. Combining these features with photoswitchable architectures offers untapped potential for reversible substrate binding and control of transition metal properties. Here, we demonstrate that the incorporation of a photoswitchable Lewis acid into intramolecular phosphorus\/boron Lewis pairs allows for stimuli\u2010responsive modulation of ambiphilicity. In the context of FLP\u2010type reactivity, both thermodynamic and kinetic control over substrate activation is achieved, culminating in the light\u2010gated binding and release of CO\n                    <jats:sub>2<\/jats:sub>\n                    . Implementing these ambiphiles as ligands in transition metal chemistry enables control over metal\u2010boron Z\u2010type interactions. Photoswitchable ambiphilicity thus provides a common light\u2010addressable handle for controlling substrate\u2010binding thermodynamics, reaction kinetics, and transition\u2010metal electronic structure.\n                  <\/jats:p>","DOI":"10.1002\/anie.5038244","type":"journal-article","created":{"date-parts":[[2026,9,24]],"date-time":"2026-09-24T07:38:21Z","timestamp":1790235501000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Photoswitchable Ambiphilicity: Light\u2010Gated Frustrated Lewis Pair Reactivity and Z\u2010Type Interaction"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-3129-7399","authenticated-orcid":false,"given":"Lennart","family":"Stoess","sequence":"first","affiliation":[{"name":"Anorganisch\u2010Chemisches Institut Ruprechts\u2010Karls Universit\u00e4t Heidelberg  Heidelberg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-2377-0087","authenticated-orcid":false,"given":"Emil L. 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