Aluminum buffer layer is introduced to improve copper crystallinity and reduce thermal stress in the electrode films. The prepared Al-Cu flexible conducting electrodes exhibit high electrical conductivity of 3.05 μΩ·cm. Negligible changes of electrical resistivity for Al(0.86 μm)-Cu thin film is achieved at the bending radius more than 6 mm. The crack evolution is effectively alleviated in Al(0.86 μm)-Cu thin film resulting from better energy recovery capacity. The Al(0.86 μm)-Cu flexible thin-film electrode exhibits strong adhesive ability to 5B-level with polyimide substrate.