We present a systematic study of the static electric hyperpolarizability of Ga2As2. The authors rely on finite-field high-level ab initio calculations with carefully optimized basis sets. Their best values for the mean and the anisotropy of the dipole polarizability are ᾱ=58.57 and Δα=130.33e2a0 2E h -1. For the hyperpolarizability we propose an estimate γ̄=(155±15) × 103e4a 0 4Eh -3, which does not agree with the negative value predicted by Lan et al. [J. Chem. Phys. 124, 094302 (2006)]. Density functional theory based methods yield values close to those predicted by conventional ab initio methods. The (hyper)polarizability components are particularly enhanced along the direction defined by the Ga-Ga axis. © 2007 American Institute of Physics.