Two interatomic potentials of the He–Kr mixture are empirically developed from the BFW and MTT type potentials by fitting them to the thermophysical and transport properties over a wide temperature range. The vector part b1 and septor part b3 of the interaction hyperpolarizability tensor of the He–Kr pair are obtained on the basis of several ab initio methods as functions of the interatomic distance. The collision-induced hyperRayleigh scattering (CIHRS) spectra scattered by the He–Kr pairs at room temperature are calculated in absolute units for the two proposed potentials and other potentials from the literature. The spectral moments are used as a criterion of the reliability of the computed profiles. The frequency-dependent depolarization ratio of the CIHRS spectra is evaluated. The spectral features of the CIHRS profiles due to b1 and b3 are discussed.