Si-MCM-41 and Al-MCM-41 with different Al contents (Si/Al = 43.9, 23.3 and 14.3) have been prepared using cetyl trimethylammonium bromide as an organic surfactant and characterised by XRD, MAS NMR and N-2 sorption studies. The transformation of cyclohexanone oxime into epsilon-caprolactam has been studied over these molecular sieves. The influences of temperature and feed rate (WHSV) on the yield of caprolactam over the samples have been investigated at different times on stream. The studies reveal that activity and selectivity increase with Al content (investigated upto Si/Al = 14) and maximum yield of epsilon-caprolactam is obtained at similar to360degreesC. (C) 2002 Elsevier Science B.V. All rights reserved.