Polymer-bound Schiff-base ligand (PS-SalPhe) was prepared from polystyrene-bound salicylaldehyde and phenylalanine, and its complex (PS-SalPhe-M) (M ϭ Co, Mn) was also synthesized. The polymer ligand and its complex were characterized by infrared spectra, small area X-ray photoelectron spectroscopy, and ICP-AES. In the presence of the complex, cyclohexene can be effectively oxidized by molecular oxygen without a reductant. The major products of the reaction are 2-cyclohexen-1-ol (-OH), 2-cyclohexen-1-one (CAO), and 2-cyclohexen-1-hydroperoxide (-OOH ), which is different from the typical oxidation of cyclohexene. The mechanism of cyclohexene oxidation is also discussed. Long-chain linear aliphatic olefins, such as 1-octene, 1-decene, 1-dodecene, and 1-tetradecene, can be directly oxidized by molecular oxygen catalyzed by PS-SalPhe-M (M ϭ Mn, Co), which yields the 1,2-epoxy alkane.