Chitosan films were prepared by casting from its 1% (w/w) solution. Tensile strength (TS), tensile modulus (TM), and elongation at break (Eb%) of chitosan films were found to be 30 MPa, 450 MPa, and 8%, respectively. Silane monomer (3-aminopropyl tri-methoxy silane) (17%, w/w) was added into the chitosan solution (1%, w/w), and films were casted. The highest TS (38 MPa) and TM (620 MPa) values were found at 5% (w/w) silane content films. Polycaprolactone (PCL) films were prepared by compression molding; the values of TS, TM, and Eb of PCL films were found to be 12 MPa, 226 MPa, and 70%, respectively. Using chitosan and silane containing chitosan films, PCL-based tri-layer films were prepared by compression molding. Chitosan (also silane-incorporated chitosan) content in the tri-layer films varied from 10 to 50% by weight. The values of TS and TM of the silane containing composites were found to be 21 and 410 MPa, respectively, which is significantly higher (40% TS and 34% TM) than control composites. Molecular interactions due to silane addition were supported by FT-IR analysis. The surface of the films and the interface of the tri-layer films were investigated by scanning electron microscope (SEM). (C) 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012