We prepared a series of blend membranes by blending waterborne polyurethane (WPU) and carboxymethylchitin (CMCH) in aqueous systems. The effects of CMCH content on the miscibility, morphology, thermal stability, and mechanical properties of the blend membranes were investigated by dilute solution viscometry (DSV), Fourier transform infrared spectroscopy, wide-angle X-ray diffraction (WXRD), scanning electron microscopy, dynamic mechanical analysis (DMA), thermogravimetric analysis, ultraviolet (UV) spectroscopy, and tensile testing. The miscibility parameter of the WPU/CMCH aqueous solution obtained by DSV predicted that the blends of WPU and CMCH were miscible or partially miscible. Moreover, the partial miscibility of the blend membranes over the entire composition range were confirmed by FTIR, WXRD, DMA, and UV spectroscopy to support the conclusion from DSV. New hydrogen bonds were formed between CMCH and WPU in the blend membranes, resulting in strong intermolecular interactions. By inducing the CMCH, we improved the tensile strength, thermostability, and organic solvent resistance of the blend membranes significantly. Therefore, this study not only provided a novel way to prepare an environmentally-friendly material but also expanded the application of chitin and CMCH. (C) 2003 Wiley Periodicals, Inc.