Abstract Fe(NO3)3/4-OH-TEMPO catalyst system was developed using the inexpensive organocatalyst 4-hydroxy-2,2,6,6-tetramethyl-piperidyl-1-oxy (4-OH-TEMPO) and the co-catalyst Fe(NO3)3·9H2O. The catalytic molecular-oxygen-driven oxidation of a broad range of primary and secondary alcohols, which may contain carbon-carbon double bond, N, O, and S heteroatoms, to the corresponding aldehydes and ketones was investigated. The results showed that reaction is highly selective to the desired products when carried out at room temperature in ambient atmosphere air. The mechanism for the catalytic aerobic oxidation of alcohols by Fe(NO3)3/4-OH-TEMPO was discussed.