Treatment of [(COT)Nd(THF)(2)(mu-Cl)](2) with dilithium tetraphenyldisiloxanediolate, (LiOSiPh(2))(2)O, in a molar ratio of 1 : 4 afforded the novel organic/inorganic triple-decker complex (mu-eta(8):eta(8)-COT)[Nd{(Ph(2)SiO)(2)O}(2){Li(THF)(2)}{Li(THF)}](2) (1) which was structurally characterized by X-ray diffraction.