LAUSR

Charge‐transfer phenomena at heterointerfaces are a promising pathway to engineer functionalities absent in bulk materials but can also lead to degraded properties in ultrathin films. Mitigating such undesired effects with an interlayer reshapes the interface architecture, restricting its operability. Therefore, developing less‐invasive methods to control charge transfer will be beneficial. Here, an appropriate top‐interface design allows for remote manipulation of the charge configuration of the buried interface and concurrent restoration of the ferromagnetic trait of the whole film. Double‐perovskite insulating ferromagnetic La2NiMnO6 (LNMO) thin films grown on perovskite oxide substrates are investigated as a model system. An oxygen‐vacancy‐assisted electronic reconstruction takes place initially at the LNMO polar interfaces. As a result, the magnetic properties of 2–5 unit cell LNMO films are affected beyond dimensionality effects. The introduction of a top electron‐acceptor layer redistributes the electron excess and restores the ferromagnetic properties of the ultrathin LNMO films. Such a strategy can be extended to other interfaces and provides an advanced approach to fine‐tune the electronic features of complex multilayered heterostructures.