The performance of polarization consistent basis sets at the Hartree-Fock and the density functional levels of theory was analyzed. The performance was evaluated in terms of 95 atomization energies, 42 ionization potentials and 10 molecular relative energies. Total atomization energies for molecules with an accuracy of better than 0.01 kJ/mol per atom were obtained. The step up in basis set quality was found to decrease the error relative to the infinite basis set limit by approximately an order of magnitude. The pc-n basis sets were found to provide better accuracy for a similar or a smaller number of basis functions.