Here, we report a method of fabricating thin layer of polydimethylsiloxane (PDMS), with a thickness in the range of 60-80 nm, which can be repeatedly generated (more than 10 times) from the same block of PDMS via controlled interfacial fracture. The thin layers can be transferred to various substrates by peeling off from the bulk PDMS. The cleavage is attributed to the built-in stress at the fracture interface due to plasma treatment, resulting in the repetitive formation of the thin membranes, with no residue from processing, and with a surface roughness of ∼5 nm. We were able to demonstrate transferred patterns with controlled thickness by varying the oxygen plasma treatment conditions and the composition of bulk PDMS stamp. Using the method, we achieved residual-free patterns with submicrometer resolution for applications in biomolecule array templates.