In this study, an efficient procedure for the synthesis of uncommon group 4-lanthanide oxo-alkoxide derivatives was developed. Heterometallic clusters with the structures [La2Ti4(mu(4)-O)(2)(mu(3)-OEt)(2)(mu-OEt)(8)(OEt)(6)(Cl)(2)(HOEt)(2)] (1), [La2Zr2(mu(3)-O)(mu-OEt)(5)(mu-Cl)(OEt)(2)(HOEt)(4)(Cl)(4)] n (2), [La2Hf2(mu(3)-O)(mu-OEt)(5)(mu-Cl)(OEt)(2)(HOEt)(4)(Cl)(4)](n) (3), [Nd2Ti4(mu(4)-O)(2)(mu(3)-OEt)(2)(mu-OEt)(8)(OEt)(6)(HOEt)(2)(Cl)(2)] (4), [Nd4Zr4(mu(3)-O)(2)(mu-OEt)(10)(mu-Cl)(4)(OEt)(8)(HOEt)(10)(Cl)(2)] (5), and [Nd4Hf4(mu(3)-O)(2)(mu OEt)(10)(mu-Cl)(4)(OEt)(8)(HOEt)(10)(Cl)(2)] (6) were synthesized via the reaction of a metallocene dichloride, Cp2M' Cl-2 (where M' = Ti, Zr, and Hf), and metallic lanthanum or neodymium in the presence of excess ethanol. This procedure gave crystalline precursors with molecular stoichiometries suitable for obtaining group 4-lanthanide oxide materials. Compounds 1-6 were examined by analytical and spectroscopic techniques and single-crystal X-ray diffraction. The magnetic properties of 5 and 6 were investigated by using direct and alternating current (dc and ac) susceptibility measurements. The results indicated weak antiferromagnetic interactions between Nd-III ions and a field-supported slow magnetic relaxation. Lanthanum-titanium compound 1 decomposed at 950 degrees C to give the perovskite compound La0.66TiO3 and small amounts of rutile TiO2. Under the same conditions, 4 decomposed to give a mixture of Nd4Ti9O24 and Nd0.66TiO3. When 4 was calcined at 1300 degrees C, decomposition of Nd4Ti9O24 to Nd0.66TiO3 and TiO2 was observed. Calcination of 2, 3, 5, and 6 at 950-1500 degrees C led to the selective formation of heterometallic La2Zr2O7, La2Hf2O7, Nd2Zr2O7, and Nd2Hf2O7 phases, respectively.