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In the field of spintronics, electric-field modulation of magnetic transition temperature and magnetic anisotropy has been studied for this purpose. An effective way to modulate the magnetic properties of correlated electron systems is electron filling control by field-effect transistor (FET). However, the application of FET systems is inevitably limited to thin films or material interfaces because of the electrostatic screening effect by electric-field-induced carriers at the materials interfaces, which prevents electric fields penetration into bulk materials. In this research, we attempt to realize an electrical control of magnetism in bulk systems by using the charge storage technique of ionics device as the filling control method. In particular, we are trying reversible magnetic phase switching through radical spins generation/annihilation by using a Li ion battery (LIB) system. Since the electronic states induced by this method are in the electrochemical equilibrium, we can expect non-volatile magnetic phase, which is maintained without continuous electric power supply. Magnetic control via ion transport accompanying redox reaction has recently been called as “Magneto-ionic control” and been attracting much attention. Reversible electrical magnetism control via radical spin generation/annihilation by using a LIB system. 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