Anisotropic anharmonicity dictates the thermal conductivity of β-Ga2O3

β-Ga2O3 is a promising material candidate for next-generation high-power devices even as its low thermal conductivity (κ) limits utilization due to an inability to sufficiently dissipate heat. Despite the importance of this inherent thermal challenge, a significant discrepancy persists between experimental results and computational models regarding the anisotropic thermal conductivity of β-Ga2O3. Specifically, computational results are within experimental error bounds for κ100 and κ001 while underpredicting κ010, suggesting that the bare phonon models used in the literature are missing essential physics related to the anisotropic thermal transport. In response, we compute the anisotropic κ using first principles and the Peirels-Boltzmann transport equation under different approximations. For the simplest model, we consider the heat carriers to be harmonic phonons with scattering rates obtained perturbatively. These results are then compared with those obtained by including phonon renormalization and four-phonon scattering. Our results show that accounting for phonon renormalization resolves the discrepancy between experiment and theory. This is because phonon renormalization leads to an anisotropic κ enhancement caused by directionally dependent changes in the phonon group velocities accompanied by a general increase in phonon lifetime. Owing to the crucial role of these anharmonic interactions in accurately describing anisotropic thermal transport, we also explore the anharmonicity of individual atoms and show that the octahedrally coordinated gallium atom is the most anharmonic and thus most likely responsible for the failure of the harmonic phonon model to describe thermal transport in this material. Finally, we demonstrate that atomic anharmonicities could be used as a useful metric to guide the tailoring of vibrational properties. © 2025 American Physical Society.