AbstractIn general, in thermoelectric materials the electrical conductivity σ and thermal conductivity κ are related and thus cannot be controlled independently. Previously, to maximize the thermoelectric figure of merit in state-of-the-art materials, differences in relative scaling between σ and κ as dimensions are reduced to approach the nanoscale were utilized. Here we present an approach to thermoelectric materials using tin disulfide, SnS₂, nanosheets that demonstrated a negative correlation between σ and κ. In other words, as the thickness of SnS₂ decreased, σ increased whereas κ decreased. This approach leads to a thermoelectric figure of merit increase to 0.13 at 300 K, a factor ∼1,000 times greater than previously reported bulk single-crystal SnS₂. The Seebeck coefficient obtained for our two-dimensional SnS₂ nanosheets was 34.7 mV K⁻¹ for 16-nm-thick samples at 300 K.