The carboxyl-terminated butadiene-a-acrylonitrile rubber (CTBN) has been proved to be the most effective toughener for cyanate ester (CE) resin. This work mainly focuses on the different modification effects caused by the addition of CTBN with different acrylonitrile content. The phase separation, morphology of fracture surface, and physical properties of the blends are studied by scanning electron microscopy (SEM), transmission electron microscopy (TEM), dynamic mechanic analysis (DMA), and thermogravimetric analysis (TGA). It is testified that the compatibility and toughness between CE and CTBN had a positive correlation with the acrylonitrile content of CTBN. (c) 2007 Wiley Periodicals, Inc.