This work is to consider the thermoelectric effect based on the vertically aligned carbon nanotube carpets (VACNTs) and vertically aligned iron-filled CNTs (Fe-filled VacNts) have been grown using a chemical vapor deposition (CVD) method. The results show the Seebeck coefficient can be improved by controlling the layer number of Fe-filled VACNTs. It found the Seebeck coefficient of the single layer Fe-filled VACNTs is approximately -65 μV/K at 120 °C, which is two times higher than that of non Fe-filled VACNTs. Briefly, this work presented a simple method for producing thermoelectric materials with well Seebeck coefficient performance.