The rapid rise in energy demand in the past years has prompted a search for low-cost alternatives for energy storage, supercapacitors being one of the most important devices. It is shown that a dramatic enhancement (≈1100%, from 155 to 1850 F g−1) of the specific capacitance of a hybrid stimuli-responsive FeNi3-graphene electrode material can be achieved when the charge/ discharge cycling is performed in the presence of an applied magnetic field of 4000 G. This result is related to an unprecedented magnetic-field-induced metal segregation of the FeNi3 nanoparticles during the cycling, which results in the appearance of small Ni clusters (<5 nm) and, consequently, in an increase in pseudocapacitive sites. The results open the door to a systematic improvement of the capacitance values of hybrid supercapacitors, while moving the research in this area towards the development of magnetically addressable energy-storage devices.