A least-squares approach has been used to determine multiplicative scaling factors for harmonic vibrational frequencies to facilitate comparison with experimentally observed frequencies. The harmonic frequencies were calculated using several of the most popular quantum chemical methods (HF, MP2, and B3LYP) and, the correlation consistent family of basis sets (cc-pVxZ and aug-cc-pVxZ, where x = D(2), T(3), or Q(4)). Calculations were performed on 41 organic molecules for which fundamental frequencies are well established. When the derived scaling factors are applied, the percentage of calculated frequencies that deviate less than 3% from the experimental frequencies is 93-97% for B3LYP and 88-92% for MP2 when quadruple-zeta level basis sets are used. Similarly, scaling factors were determined for computing the vibrational components of the thermal contributions to enthalpy and entropy. An additional set of molecules was used in calculating scaling factors for the zero-point vibrational energy.