In single-component homogeneous nucleation, the summation expression for the steady-state nucleation rate requires values of the forward rate constants and Gibbs free energies of cluster formation. If atomistic data are available for these quantities, then these could be used instead of CNT. In an atomistic approach, clusters are treated as distinct molecular species, rather than as a small piece of the bulk condensed phase. Examples are presented of atomistic data generated by means of computational chemistry for water clusters up to size 10, and for aluminum clusters up to size 60. In both cases, the free energy of cluster formation is found to be a multimodal function of cluster size, both quantitatively and qualitatively different than in CNT. Condensation rate constants can be affected by the need for a third body as a collision partner, and by attractive intermolecular forces in collisions between clusters and monomers. An approach is suggested for constructing a “master table” of free energies of cluster formation, based on a hybrid of atomistic data, experimental values inferred by means of the nucleation theorem, and extrapolations to larger cluster sizes based on CNT.