The blends of high molecular weight poly(propylene carbonate) (PPC) and poly(butylene succinate) (PBS) were melt blended using triphenylmethane triisocyanate (TTI) as a reactive coupling agent. TTI also serves as a compatibilizer for the blends of PPC and PBS. The blend containing 0.36 wt % TTI showed that the optimal mechanical properties were, therefore, calendared into films with different degrees of orientation. The calendering condition, degree of orientation, morphologies, mechanical properties, crystallization, and thermal behaviors of the films were investigated using wide-angle X-ray diffraction, scanning electron microscopy, tensile testing, and differential scanning calorimetry (DSC) techniques. The result showed that the as-made films exhibited obvious orientation in machine direction (MD). Both tensile strength in MD and the tear strength in transverse direction (TD) increased with increasing the degree of orientation. The orientation of the film also increased the crystallinity and improved the thermal properties of the PPC/PBS blend films. (C) 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 128: 390-399, 2013