An intermediate neglect of differential overlap method for examining the electronic structure of actinide complexes is developed. It is characterized by a basis set obtained from relativistic Dirac-Fock atomic calculations, the inclusion of all one-center two-electron integrals, and a parameter set based on molecular geometry and ionization spectra. The model is successful in reproducing the geometries of many small test molecules, especially the hexahalides and tetrahalides of the early actinides. We also investigate the bonding in actinocenes and the photoelectron spectra of pentavalent uranium amide/imide complexes as two diverse examples in which this model can be used to help in understanding and prediction.