A series of cyano-containing polyimides were synthesized from 2,6-bis(4-aminophenoxy) benzonitrile and some aromatic dianhydride monomers by solution polycondensation. The poly(amic acid) films could be obtained by solution-cast from N-methyl-2- pyrrolidinone solutions and thermally converted into tough polyimide films. Structure and physical properties of thin films of those polyimides were measured by FTIR, TGA, dynamic mechanical analysis and LCR hitester et al. Results showed that the polyimides prepared from 2,6-bis(4-aminophenoxy)benzonitrile and 2,2-bis[4-(3,4-dicarboxyphenoxy) phenyl] propane dianhydride or 4,4'-(hexafluoropropylidene) diphthalic anhydride exhibited more excellent energy-damping characteristic and excellent solubility in NMP, DMF, DMAc, DMSO, THF and CHCl3, whereas the polyimides from 2,6-bis( 4-aminophenoxy) benzonitrile and 3,3', 4,4'-biphenyltetracarboxylic dianhydride or Pyromellitic dianhydride were insoluble in polar and nonpolar organic solvents. All polyimides indicated higher glass transition temperatures, excellent thermal stability and tensile properties. Incorporating a nitrile group into the polyimide backbone would enhance the dielectric constant of the polyimide films.