Two pyridine dipyrrolide neptunium(IV) complexes, (MesPDPPh)NpCl2(THF) and Np(MesPDPPh)2, where (MesPDPPh)2– is the doubly deprotonated form of 2,6-bis(5-(2,4,6-trimethylphenyl)-3-phenyl-1H-pyrrol-2-yl)pyridine, have been prepared. Characterization of the complexes has been performed through a combination of solid- and solution-state methods, including single-crystal X-ray diffraction and electronic absorption and nuclear magnetic resonance spectroscopies. Collectively, these data confirm the formation of the mono- and bis-ligated species. Electrochemistry of a series of bis-ligated actinide complexes, An(MesPDPPh)2 (An = Th, U, Np), is presented.