The objective of this study was to investigate the effect of methyldiphenyl diisocyanate (MDI) concentration (0, 0.2, 1, 2, and 3%) on the wettability and adhesion of blend solutions of poly(lactic acid) (PLA) and chitosan (CS) when coated on PLA film for development of a bio-based multi-layer film suitable for food packaging and other applications. Characterization was carried out by attenuated total reflectance infrared spectrometry (ATR-FTIR), contact angle (theta), mechanical adhesion pull-off testing, and scanning electron microscopy (SEM). The theta of the PLA/CS blend shifted to a lower value (41-35 degrees) with increasing MDI concentration showing that the surface tension was modified between the PLA/CS blend solution and PLA film and better wettability was achieved. The increase in MDI also resulted in an increased breaking strength (228-303 kPa) due to the increased H-bonding resulting from the more urethane groups formed within the PLA/CS blend as shown by ATR-FTIR. The improved adhesion was also shown by the increased number of physical entanglements observed by SEM. It can be concluded that MDI can be used to improve wettability and adhesion between PLA/CS coating and PLA film. (C) 2015 Elsevier B.V. All rights reserved.