Electric-field-gradient (EFG) tensors, at the zinc nuclear site were calculated using quantum mechanical methods for a series of zinc(H) coordination complexes. The accuracy of the calculated Zn-67 EFG results at restricted Hartree-Fock (RHF) and density functional theory (DFT) levels was evaluated by comparing them with experimental solid-state Zn-67 NMR data. Theoretical Zn-67 EFG results at the B3LYP level using medium basis sets of 6-31G(f) for Zn and 6-31G(d) for ligand atoms were in good agreement with experimental Zn-67 NMR data.