As the number of flexible electronic devices grows dramatically, the energy harvesting and storage technology of flexible electronic devices also urgently needs to advance. Traditional flexible electronic devices are battery-powered, which not only suffer from short endurance and large size, but also do not meet the new era requirement of environmental protection and energy saving. Therefore, this study investigates the self-powered system in flexible electronic devices using the Triboelectric Nanogenerator (TENG) technology. The research innovatively optimizes the TENG, proposes a liquid metal triboelectric Nanogenerator (LMTENG), and optimizes the optimal path selection problem. In the test results, the optimal output power of 567.3 μW is obtained when the contact frequency is 2 Hz for an external load of 15 MΩ. By comparing with the current TENG, the LMTENG significantly improves the optimal output power. On the other hand, the LMTENG is able to respond to a pressure of 22 kPa and maintain normal performance at 50% stretching. The study provides new ideas for improvement of triboelectric nanogenerators and also contributes to the optimization of flexible electronic devices.