First‐principles calculations were carried out to investigate the synthesized orthorhombic CrB4. Our calculations show that the shear modulus of orthorhombic CrB4 is much higher than that of superhard WB4. Moreover, its shear modulus is larger than its bulk modulus. Boron atoms in CrB4 form a strong covalent cage which dramatically increases its mechanical strength. The calculated elastic constants imply that CrB4 is elastically stable. The calculated density of states shows that CrB4 is metallic. The appearance of pesudogap near the Fermi level means that CrB4 is a stable compound. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
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