It is shown how the regularized two-component relativistic Hamiltonians of Heully et al. and Chang, Pelissier, and Durand can be viewed as arising from a perturbation expansion that unlike the Pauli expansion remains regular even for singular attractive Coulomb potentials. The performance of these approximate Hamiltonians is tested in the framework of the local density approximation and the relation of their spectrum to that of the Dirac Hamiltonian is discussed. The circumstances under which the current approximations are superior to the Pauli Hamiltonian are analyzed. Finally, it shown how the Hamiltonians could be used within the context of conventional Hartree-Fock theory. © 1996 John Wiley & Sons, Inc.