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In this paper, we have studied the relevant physical quantities to the figure of merit of carbon nanotube (CNT)/polydimethylsiloxane composites at different loadings, and found that with increasing the CNT loadings, the electrical conductivity jumps several orders in magnitude at ‘threshold’, followed by a saturated plateau, and the Seebeck coefficient decreases by a small margin, and the thermal conductivity increases somewhat. According to the formula of the figure of merit, it is found that higher loading composites display a larger figure of merit. We hope the present study provides a new path to high-performance flexible thermoelectric materials.