Orange peel-derived pectin jelly/corn starch-based biocomposite films with and without layered silicates (LSs) were prepared using melt extrusion followed by film die casting. To enhance interfacial compatibility, corn starch and LSs were chemically modified. Regardless of chemical modification or LS weight content, different pectin jelly-to-starch weight ratios (63/37, 60/40, 57/43, and 54/46) were considered to formulate the ingredients of biocomposite films in light of Taguchi-based predictions. X-ray diffraction (XRD), fourier transform infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), thermal gravimetric analysis (TGA), scanned electron microscopy (SEM) and transmission electron microscopy (TEM) were systematically used to characterize corn starch, LSs, and biocomposite films. Among all the films considered, pectin jelly/modified (15%) starch-based biocomposite film (54/46 w/w) containing 0.25 wt % of pristine LSs was found to be the most promising in terms of texture structure and mechanical integrity. Furthermore, creep recovery, hydrophobicity, and water vapor and oxygen gas transmission rates of the most promising biocomposite film were experimentally determined. Based on the findings obtained, the overall performance of the biocomposite film was evaluated and weighed against the overall performance of a low-density polyethylene film. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40654.