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A semi-flexible binder-free graphitic carbon nitride (g-C3N4) intercalated polypyrrole (PPy) nanocomposite thin film was prepared via hybrid electrospray technique. A homogeneous thin film was achieved by the controlled spray process. A deposited thin film illustrated the amorphous nature of composite with high surface purity and good chemical composition. The surface analysis confirmed the smoother surface with well-defined distinct phases of g-C3N4 and PPy matrix in the composite thin film. The electrochemical studies exhibited that a maximum areal capacity of the thin film was achieved to be 289.6 mF/cm2 at a current density of 0.4 mA/cm2, which is higher than that of pristine PPy (194.8 mF/cm2). The heterostructure electrode illustrated that the life cycles of 99％could be up to 10,000 cycles with low resistance due to the synergetic effect of g-C3N4 and PPy matrix with strong material adhesion (hybrid spray process) on the surface. A binder-free heterostructure thin film will play a significant role in the energy storage application.