The computationally most efficient lrWFT-srDFT model will be for the smallest µ value for which long-range and spin correlations can be described to the desired accuracy, as this leads to the most compact lrWFT part with the smallest number of active orbitals. By comparison with accurate WFT calculations, it has been found that a value around µ = 0.4 can be considered universally applicable for valence properties of singlet molecules. Preliminary investigations of transition-metal complexes indicate that a value around µ = 1.0 may be needed to describe their spin correlation sufficiently well. A particularly promising choice for the lrWFT part is to use the variational multiconfigurational self-consistent field description, leading to an lrMCSCF-srDFT (MC-srDFT) model. Because it is variational, the MC-srDFT model can also be used for molecular response properties, just like TDDFT in Kohn-Sham DFTnot only for excitation energies and transition moments, but in general for optical, electrical, and magnetic perturbations. For molecules with strong nondynamical correlation, the kinetic energy will be better described with the MC-srDFT model than with Kohn-Sham-DFT, thus a smaller kinetic-energy correction needs to be described by the correlation functional.