The C-13, N-15, O-17, and S-33 chemical shieldings for three optimized structures of hypothiocyanite have been calculated at the SCF, MP2, and CCSD levels using the gauge-including atomic-orbital approach. The first few excitation energies for the corresponding hypothiocyanous acids have been obtained using the equation-of-motion CCSD and the CI singles methods. Comparison of the calculated N-15 chemical shifts and of the excitation spectra with experimental data suggests that hypothiocyanite has a bent OSCN- structure with C-s symmetry, even though the linear SNCO- isomer is 86 kJ/mol lower in energy. The linear ONCS- structure is 146 kJ/mol above SNCO-. No other low-lying structures were found.