so far, mainly originates from the elec tric currents utilized to control the mag netic properties. A promising alternative for increasing the energy efficiency of magnetic devices is to control the mag netism by electric fields instead of electric currents. This possibility has triggered intense research into magnetoelectric materials, but much of this is restricted to low temperature and high voltage opera tion and/or complex layer synthesis. [1] More recently, magnetoelectric appro aches involving the voltagegating of mag netic nanostructures via a dielectric oxide or an electrolyte were examined. [1-3] In these approaches, ferro and ferrimagnetic metals or oxides exhibiting Curie tem peratures above room temperature can be used and often only few volts are required during gating. The modulation of mag netic properties in voltagegated magnetic nanostructures is based on either voltage induced capacitive charging or electro chemical (magnetoionic) processes. [2-4] Voltageinduced capacitive charging of a ferromagnetic metal interface causes volatile changes in the sur face electronic band structure that affect the intrinsic magnetic properties in just a few atomic layers. [5-10] In contrast, magneto ionic mechanisms involve voltageinduced ion migration and electrochemical reactions, [2,3,11-13] and can therefore induce very large and nonvolatile magnetic property changes. [12,14-18] As a High energy efficiency of magnetic devices is crucial for applications such as data storage, computation, and actuation. Redox-based (magneto-ionic) voltage control of magnetism is a promising room-temperature pathway to improve energy efficiency. However, for ferromagnetic metals, the magnetoionic effects studied so far require ultrathin films with tunable perpendicular magnetic anisotropy or nanoporous structures for appreciable effects. This paper reports a fully reversible, low voltage-induced collapse of coercivity and remanence by redox reactions in iron oxide/iron films with uniaxial in-plane anisotropy. In the initial iron oxide/iron films, Néel wall interactions stabilize a blocked state with high coercivity. During the voltage-triggered reduction of the iron oxide layer, in situ Kerr microscopy reveals inverse changes of coercivity and anisotropy, and a coarsening of the magnetic microstructure. These results confirm a magneto-ionic deblocking mechanism, which relies on changes of the Néel wall interactions, and of the microstructural domainwall-pinning sites. With this approach, voltage-controlled 180° magnetization switching with high energy-efficiency is achieved. It opens up possibilities for developing magnetic devices programmable by ultralow power and for the reversible tuning of defect-controlled materials in general.