Ever increasing energy demand urges to impelled extensive research in the development of new eco-friendly energy harvesting and storage technologies. Energy harvesting technology exploiting renewable energy sources is an auspicious method for sustainable, autonomous, and everlasting operation of a variety of electronic devices. A new concept of an integrated self-powered system by combining an energy harvesting device with an energy storage device has been established to harvest renewable energy and simultaneously store it for sustainable operation of electronic devices. In this chapter, describes the fabrication of a self-powered system by integrating the supercapacitor with energy harvesting devices such as nanogenerator and solar cells to power portable electronic devices. Initially synthesis and electrochemical characterization of various electroactive materials for supercapacitors and further, fabrication of supercapacitor device were discussed. In conclusion, this chapter demonstrates self-powered system by the integration of energy harvesting, energy storage module with portable electronic devices. The various result validates the feasibility of using supercapacitors as efficient energy storage components in self-powered devices. The proposed self-powered technology based on energy conversion of renewable energy to electrical energy which stored in energy storage device and it will be used to operate several electronic devices as a self-powered device.