AbstractHeterogeneous selective oxidation of alcohol to carbonyl compounds with stable organic nitroxyl radicals is highly attractive yet grand challenging. Described herein is a highly promising heterogeneous strategy for this reaction in which a catalytic amount of 1‐methyl‐2‐azaadamanane N‐oxyl immobilized on magnetic polystyrene nanosphere (1‐Me‐AZADO/MPNs) was used and a series of carbonyl compounds were obtained from various alcohols in 73–99 % isolated yields and high selectivity (>99 %) under Anelli conditions, thus offering a greener and more convenient methods in the synthesis of carbonyl compounds. The attractive features of convenient magnetic separation (within seconds), good recyclability (up to 20 runs) and fast reaction rates (5–20 min) were very efficient to improve the utility of azaadamantane‐type‐nitroxyl radicals in the oxygenation.