It has been reported that single crystals of CoO2-based oxides with layered structures show good p-type thermoelectric properties. In order to realize thermoelectric power generation, n-type oxides possessing thermoelectric properties as good as CoO2-based oxides are indispensable. We are exploring new n-type oxides using a combinatorial technique, in which 1000 samples can be prepared and evaluated their thermoelectric properties a day. Aqueous solutions of metal nitrates were used as starting materials. In an hour, a single library of 100 samples can be prepared on a 100 × 100 mm alumina plate for heat treatment. Evaluation of coefficient was performed using a Seebeck tester at a rate of 600 samples/h. In the binary system, the Nd-Ni-O libraries are found out to show n-type thermoelectric properties.