In this study, nanocellulose (NC) (2-5%, w/w) and grape seed extract (GSE) (15%, w/w) added chitosan (CH) and polycaprolactone (PCL) based active bilayer films were prepared by either coating with PCL in the form of chloroform solution (C-PCL) or compression of PCL and CH layers (P-PCL). Films were tested by means of scanning electron microscopy (SEM), water vapor permeability (WVP), tensile tests, optical and active properties (antimicrobial, and antioxidant activities), and release studies. The incorporation of NC significantly reduced WVP and opacity of films while GSE addition had an adverse effect. P-PCL films showed higher elastic modulus, tensile strength and WVP values and lower elasticity when compared to C-PCL films (p < 0.05). All film samples showed antimicrobial activity, and GSE retained its antioxidant capacity within CH matrix. The formation of the CH and PCL based bilayer films with NC and GSE improved the suitability of CH films for food packaging applications.