Nature Communications, Published online: 26 June 2026; doi:10.1038/s41467-026-74846-8 While the oxidative cleavage of olefins is well established, the radical-mediated, chemo- and regioselective cleavages of allene C(sp)–C(sp2) and C(sp3)– C(sp2) bonds remain unresolved challenges in synthetic chemistry. Herein, the authors present base metal-catalyzed cleavage of allenic C(sp)–C(sp2) double bonds and C(sp3)–C(sp2) single bonds utilizing air as an oxidant.