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Abstract

A surge in interest of oxide‐based materials is testimony for their potential utility in a wide array of device applications and offers a fascinating landscape for tuning the functional properties through a variety of physical and chemical parameters. In particular, selective electronic/defect doping has been demonstrated to be vital in tailoring novel functionalities, not existing in the bulk host oxides. Here, an extraordinary interstitial doping effect is demonstrated centered around a light element, boron (B). The host matrix is a novel composite system, made from discrete bulk LaAlO₃:LaBO₃ compounds. The findings show a spontaneous ordering of the interstitial B cations within the host LaAlO₃ lattices, and subsequent spin‐polarized charge injection into the neighboring cations. This leads to a series of remarkable cation‐dominated electrical switching and high‐temperature ferromagnetism. Hence, the induced interstitial doping serves to transform a nonmagnetic insulating bulk oxide into a ferromagnetic ionic–electronic conductor. This unique interstitial B doping effect upon its control is proposed to be as a general route for extracting/modifying multifunctional properties in bulk oxides utilized in energy and spin‐based applications.