<p>The oxidation of allyl is a cornerstone for direct C–H functionalization, widely exploited in the assembly of natural products, pharmaceuticals and advanced materials. Traditional protocols that rely on highly toxic chromium- or selenium-based reagents, or costly noble-metal catalysts, are ill-suited to scale-up and industrial implementation. Herein, we demonstrate that Co-Beta zeolite, a cobaltosilicate in which isolated Co(II) sites are incorporated into the zeolite framework, can catalyze the aerobic allylic oxidation of cyclohexene under mild conditions with exceptional activity, high chemoselectivity, and robust stability. Typically, Co-Beta zeolite achieved stable cyclohexene conversion of 53% and allylic product selectivity of 85% under optimal conditions, with these results consistently observed over five cycles. The reaction mechanism of cyclohexene oxidation is investigated via the combination of spectroscopic analyses and kinetic studies. It is found that, within the Co-Beta zeolite matrix, dioxygen and cycloolefin are simultaneously activated through a radical pathway, realizing the fast and efficient conversion of cycloolefins. Built from earth-abundant Si, Al, Co and O₂, the system is inherently inexpensive and environmentally benign, which can be extended to the allylic oxidation of alkanes and other hydrocarbons without generating hazardous waste streams.</p>