Perovskite oxides ABO₃ continue to be a major focus in materials science. Of particular interest is the interplay between A and B cations as exemplified by intersite charge transfer (ICT), which causes novel phenomena including negative thermal expansion and metal-insulator transition. However, the ICT properties were achieved and optimized by cationic substitution or ordering. Here we demonstrate an anionic approach to induce ICT using an oxyhydride perovskite, EuVO₂H, which has alternating layers of EuH and VO₂. A bulk EuVO₂H behaves as a ferromagnetic insulator with a relatively high transition temperature (T_C) of 10 K. However, the application of external pressure to the Eu^IIV^IIIO₂H bulk or compressive strain from the substrate in the thin films induces ICT from the Eu^IIH layer to the V^IIIO₂ layer due to the extended empty V d_xy orbital. The ICT phenomenon causes the VO₂ layer to become conductive, leading to an increase in T_C that is dependent on the number of carriers in the d_xy orbitals (up to a factor of 4 for 10 nm thin films). In addition, a large perpendicular magnetic anisotropy appears with the ICT for the films of <100 nm, which is unprecedented in materials with orbital-free Eu²⁺, opening new perspectives for applications. The present results provide opportunities for the acquisition of novel functions by alternating transition metal/rare earth layers with heteroanions.

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