In this study, a flexible hybrid film based on single-wall carbon nanotubes (SWNTs) was fabricated. The SWNTs@MnO2/Polypyrrole (PPy) film was used as a supercapacitor electrode without binders to achieve high capacitance. The binder-free electrode with SWNT and PPy layers improved the conductivity of the electrode materials, as well as the ion diffusion rate and charge-transfer resistance, thus achieving excellent electrochemical performance compared with SWNTs@MnO2 electrodes. The specific capacity was 351Fg−1 based on the total weight of the electrodes with energy density of 39.7Whkg−1 and power density of 10kWkg−1. Our study could provide a novel and facile strategy for the development of high-performance energy storage devices.