Polycarbazole/chitosan composite materials were synthesized electrochemically at various loadings of chitosan (Chi). Their electrochemical, structural, thermal, and morphological characterizations were investigated by cyclic voltammetry, chronoamperometry, electrochemical impedance spectroscopy, Fourier transform infrared spectroscopy, thermal gravimetry, and scanning electron microscopy. Further electrical conductivity was measured using a four-point probe technique. The electrochemical results showed that the electrical conductivity of the polymeric composite film was increased by increasing the amount of Chi in the electrolyte medium. The as-prepared composite films exhibited enhanced electrical conductivity and structural properties of polycarbazole due to the presence of Chi in the composite films.