The synthesis of tetravalent thorium and uranium complexes with the phosphaazaallene moiety, [N(tBu)C=P(C6H5)]2−, is described. The reaction of the bis(phosphido) complexes, (C5Me5)2An[P(C6H5)(SiMe3)]2, An = Th, U, with two equivalents of tBuNC produces (C5Me5)2An(CNtBu)[η2-(N,C)-N(tBu)C=P(C6H5)] with concomitant formation of P(SiMe3)2(C6H5) via silyl migration. These complexes are characterized by NMR and IR spectroscopy, as well as structurally determined using X-ray crystallography.