The electric field gradient (EFG) at the nucleus, the generalized Sternheimer shielding constants, and the EFG hyperpolarizabilities of a set of reference molecules are computed using analytic density-functional (up to quadratic) response theory. At the three-parameter Becke–Lee–Yang–Parr (B3LYP) level, density functional theory (DFT) un-derestimates correlation effects compared with other approaches such as coupled-cluster and multiconfigurational self-consistent field. For the prediction of EFG properties of hydrogen nuclei and electron-rich atoms such as halides, DFT/ B3LYP provides results even less reliable than Hartree–Fock theory. Ó 2003 Elsevier Science B.V. All rights reserved.