Freestanding and robust thin-film electrodes are the basis for future renewable energy technology owing to their unique merits: i) additive-free features enable facile fabrication route and long lifetime; ii) can be easily recycled; iii) significantly reduce the weight and volume of the energy devices, especially for batteries and supercapacitors; iv) can be integrated into wearable electronic systems. However, previous efforts fail to make significant progress in freestanding metal compound thin-films due to a lack of fundamental understanding and technological breakthrough in freestanding metal compound thin-films. In this work, transformative thin-film nanomanufacturing technology has been developed to fabricate freestanding metal compound thin-films using a facile and scalable electrochemical route. Both experimental and computational studies indicate that a supreme electrochemical performance can be achieved by tuning the microstructure and composition of thin-films. Outstanding energy storage and hydrogen generation properties are therefore obtained by directly using these advanced thin-films as electrodes.