The first actinide complexes of the pyridine dipyrrolide (PDP) ligand class, (MesPDPPh)UO2(THF) and (Cl2PhPDPPh)UO2(THF), are reported as the UVI uranyl adducts of the bulky aryl substituted pincers (MesPDPPh)2- and (Cl2PhPDPPh)2- (derived from 2,6-bis(5-(2,4,6-trimethylphenyl)-3-phenyl-1H-pyrrol-2-yl)pyridine (H2MesPDPPh, Mes = 2,4,6-trimethylphenyl), and 2,6-bis(5-(2,6-dichlorophenyl)-3-phenyl-1H-pyrrol-2-yl)pyridine (H2Cl2PhPDPPh, Cl2Ph = 2,6-dichlorophenyl), respectively). Following the in situ deprotonation of the proligand with lithium hexamethyldisilazide to generate the corresponding dilithium salts (e.g., Li2ArPDPPh, Ar = Mes of Cl2Ph), salt metathesis with [UO2Cl2(THF)2]2 afforded both compounds in moderate yields. The characterization of each species has been undertaken by a combination of solid- and solution-state methods, including combustion analysis, infrared, electronic absorption, and NMR spectroscopies. In both complexes, single-crystal X-ray diffraction has revealed a distorted octahedral geometry in the solid state, enforced by the bite angle of the rigid meridional (ArPDPPh)2- pincer ligand. The electrochemical analysis of both compounds by cyclic voltammetry in tetrahydrofuran (THF) reveals rich redox profiles, including events assigned as UVI/UV redox couples. A time-dependent density functional theory study has been performed on (MesPDPPh)UO2(THF) and provides insight into the nature of the transitions that comprise its electronic absorption spectrum.