The harmonic approximation for the potential energy of proteins is known to be inadequate for the calculation of many protein properties. To study the effect of anharmonic terms on protein vibrations, the anharmonic wave functions for the ground state and low-lying excited states of the bovine pancreatic trypsin inhibitor (BPTI) were calculated. The results suggest that anharmonic treatments are essential for protein vibrational spectroscopy. The calculation uses the Vibrational self-consistent field approximation, which includes anharmonicity and interaction among modes in a mean-field sense. Properties obtained include the quantum coordinate fluctuations, zero-point energies, and the vibrational absorption spectrum.