The low-valent U(III) complexes [((t-BuArO)3mes)U] and [((AdArO)3N)U] react with CO2 to form the bridging carbonate complexes [{((t-BuArO)3mes)U}2(mu-kappa2:kappa2-CO3)] and [{((AdArO)3N)U}2(mu-eta1:kappa2-CO3)]. Uranium(IV) bridging oxo complexes have been determined to be the intermediate in these transformations.