An approach for simultaneously synthesizing and immobilizing silver nanoleaves (SNLs) on gamma-mercaptopropylttimethyoxysilane (MPTS)modified chemical vapor deposited (CVD) diamond film surface has been developed. As-grown diamond film surface was oxidized by exposing to UV irradiation in oxygen gas atmosphere, and then the oxygen-terminated diamond film was dipped into a methanol solution of MPTS to form a self-assembled MPTS monolayer on the diamond film surface. SNLs were then deposited on diamond film surfaces by an electroless process. The morphology of SNL film was characterized by scanning electron microscopy. The thickness of SNL layer deposited onto the CVD diamond substrate increased with increasing the deposition time and the formation mechanism of SNL films was also discussed. Their performance as surface-enhanced Raman scattering (SERS) substrates was evaluated by using rhodamine 6G (R6G) as the probe molecule. Compared with self-assembled silver nanoparticle film and silver film from the mirror reaction, the SERS signal of R6G was obviously improved on the SNL films. (C) 2008 Elsevier B.V. All rights reserved.