The dataset on the nuclide 66Zn was obtained from nuclear resonance fluorescence experiments at the High Intensity Gamma-ray Source of TUNL at Duke University in Durham, NC, USA. A linearly polarized and quasimonoenergetic photon beam - generated via laser Compton backscattering of relativistic electrons - was used to measure the photoresponse of 66Zn as a function of the excitation energy from 5.6 MeV to 9.9 MeV. The dataset provided contains a table with the cross sections of the electric and magnetic ground-state decay contributions, the total photoabsorption cross sections and its elastic and inelastic components as well as the measured asymmetries. All cross sections are given in units of millibarn (mb).