A unique combination of oxidant, solvent, and catalyst is proposed for the allylic and benzylic oxidation of alkenes to enones with 100% selectivity and good conversion. The proposed catalyst, CrMCM-41, in combination with H2O2 is found to be highly active and selective for this purpose. The catalyst is also found to be very useful for selective oxidation of toluene and aniline. It is also proved that the catalyst can be reused several times while maintaining its structural integrity and activity. (c) 2007 Elsevier Inc. All rights reserved.