SignificanceFerromagnetic insulators are highly needed as the necessary components in developing next-generation dissipationless quantum-spintronic devices. Such materials are rare, and those high symmetric ones without chemical doping available so far only work below 16 K. Here we demonstrate a tensile-strained LaCoO3 film to be a strain-induced high-temperature ferromagnetic insulator. Both experiments and first-principles calculations demonstrated that the tensile-strain–supported ferromagnetism reaches its strongest when the composition is nearly stoichiometric. It disappears when the Co2+ defect concentration reaches around 10%. The discovery represents a chance for the availability of such materials, a high operation temperature, and a high epitaxial integration potential for making future devices.

Engineering magnetic anisotropy in two-dimensional systems has enormous scientific and technological implications. The uniaxial anisotropy universally exhibited by two-dimensional magnets has only two stable spin directions, demanding 180° spin switching between states. We demonstrate a previously unobserved eightfold anisotropy in magnetic SrRuO3 monolayers by inducing a spin reorientation in (SrRuO3)1/(SrTiO3)N superlattices, in which the magnetic easy axis of Ru spins is transformed from uniaxial 〈001〉 direction (N < 3) to eightfold 〈111〉 directions (N ≥ 3). This eightfold anisotropy enables 71° and 109° spin switching in SrRuO3 monolayers, analogous to 71° and 109° polarization switching in ferroelectric BiFeO3. First-principle calculations reveal that increasing the SrTiO3 layer thickness induces an emergent correlation-driven orbital ordering, tuning spin-orbit interactions and reorienting the SrRuO3 monolayer easy axis. Our work demonstrates that correlation effects can be exploited to substantially change spin-orbit interactions, stabilizing unprecedented properties in two-dimensional magnets and opening rich opportunities for low-power, multistate device applications.