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Abstract Point defects typically reduce the thermal conductivity (κ) of a crystal due to increased scattering of heat‐carrying phonons, a mechanism that is well understood and widely used to enhance or impede heat transfer in the material for different applications. Here an opposite effect is reported where the introduction of point defects in graphite with energetic particle irradiation increases its cross‐planeκby nearly a factor of two, from 10.8 to 18.9 W m K⁻¹at room temperature. Integrated differential phase contrast imaging with scanning transmission electron microscopy revealed the creation of spiro interstitials in graphite by the irradiation. The enhancement inκis attributed to a remarkable mechanism that works to the benefit of phonon propagation in both the harmonic and anharmonic terms: these spiro interstitial defects covalently bridge neighboring basal planes, simultaneously enhancing acoustic phonon group velocity and reducing phonon–phonon scattering in the graphite structure. The enhancement ofκreveals an unconventional role of lattice defects in heat conduction, i.e., easing the propagation of heat‐carrying phonons rather than impeding them in layered materials, inspiring their applications for thermal management in heavily radiative environments. 

Abstract 2D layered materials have emerged in recent years as a new platform to host novel electronic, optical, or excitonic physics and develop unprecedented nanoelectronic and energy applications. By definition, these materials are strongly anisotropic between the basal plane and cross the plane. The structural and property anisotropies inside their basal plane, however, are much less investigated. Black phosphorus, for example, is a 2D material that has such in‐plane anisotropy. Here, a rare chemical form of arsenic, called black‐arsenic (b‐As), is reported as a cousin of black phosphorus, as an extremely anisotropic layered semiconductor. Systematic characterization of the structural, electronic, thermal, and electrical properties of b‐As single crystals is performed, with particular focus on its anisotropies along two in‐plane principle axes, armchair (AC) and zigzag (ZZ). The analysis shows that b‐As exhibits higher or comparable electronic, thermal, and electric transport anisotropies between the AC and ZZ directions than any other known 2D crystals. Such extreme in‐plane anisotropies can potentially implement novel ideas for scientific research and device applications.