Dia- and paramagnetic shielding constants of HF, NH3, N2, H2O, and CO were calculated in the 4-31G, 4-31G*, and 6-31G** bases, using gauge-invariant atomic orbitals. Correlation effects were evaluated by 2nd-order perturbation theory: while the diamagnetic contributions are virtually unaffected by correlation, the paramagnetic parts (σρ) are modified by ~10 ppm in the 6-31G** basis. With or without correlation, calculated σρ values differ significantly from results obtained from measured spin-rotation constants. However, improvements in the basis set descriptions and inclusion of correlation yield chemical shift values for 15N and 17O converging toward their experimental counterparts obtained from conventional nuclear magnetic resonance spectroscopy.