Polycarbazole (PCz) was synthesized by chemical polymerization of carbazole in acetonitrile medium using ammonium persulfate as oxidant. The selection of solvent, concentration of the monomer, composition of the solvent, polymerization time, temperature, and pH were optimized to obtain better quality and yield of the polycarbazole. The synthesized polycarbazole was characterized by various techniques such as UV-Visible, FTIR, H-1-NMR, C-13-NMR, COSY, NOESY, and XRD spectroscopy. The solubility of the polycarbazole was tested in various solvents. The thermodynamic stability of the polycarbazole was examined by DSC and TGA-DTA analysis. (C) 2009 Wiley Periodicals, Inc. J Appl Polym Sci 116: 147-154, 2010