The ability to tailor a new crystalline structure and associated functionalities with a variety of stimuli is one of the key issues in material design. Developing synthetic routes to functional materials with partially absorbed non-metallic elements (i.e., hydrogen and nitrogen) could open up more possibilities for preparing novel families of electronically active oxide compounds. Here, we introduce a fast and reversible uptake and release of hydrogen in epitaxial ABO3 manganite films through an adapted low-frequency inductively coupled plasma technology. Compared with traditional dopants of metallic cations, the plasma-assisted hydrogen implantations not only produce reversibly structural transformations from pristine perovskite (PV) phase to a newly found protonation-driven brownmillerite (BM) one, but also regulate remarkably different electronic properties driving the material from a ferromagnetic metal to a weakly ferromagnetic insulator for a range of manganite(La1-xSrxMnO3) thin films. Moreover, a reversible perovskite-brownmillerite-perovskite (PV-HBM-PV') transition is achieved at a relatively low temperature (T ≤ 350°C), enabling multi-functional modulations for integrated electronic systems. The fast, low-temperature control of structural and electronic properties by the facile hydrogenation/dehydrogenation treatment substantially widens the space for exploring new possibilities of novel properties in proton-based multifunctional materials.