batteries that need frequent recharging and/or replacing. [1-3] Harvesting thermal energy is particularly attractive as there are abundant environmental heat sources and most of them, such as the heat released by exhausts, industrial processes, and radiators, or even that arising from human body heat, are mostly unexploited. [4] Thermoelectric generators (TEGs) based on thermoelectric (TE) materials are prime candidates for thermal energy harvesting due to their ability to convert ambient and ever-present waste heat into electrical energy by utilizing the Seebeck effect. [5] TEGs have the potential to be scaled down in size and integrated into self-powered electronic devices with minimal maintenance. [6] However, a problem faced in this field is that existing inorganic TE materials often suffer from scarcity and/or toxicity. Furthermore, it is difficult to scale up the production of many of these materials, which are often not suitable for flexible and/or conformable applications due to their rigid nature. Accordingly, it is important for the future of this technology that new classes of TE materials are developed and evaluated. In order to evaluate the performance of TE materials, the dimensionless figure of merit (ZT) is usually used to describe their potential energy conversion efficiency. For a given operating temperature, ZT is defined as ZT = S 2 σT / κ, where T is the temperature, κ is the thermal conductivity (W (m K) −1), σ is the electrical conductivity (S m −1), and S is the Seebeck coefficient (V K −1). [7,8] A good TE material therefore needs to possess a high S and σ to ensure a high-voltage output at a given temperature difference. The power factor (PF = S 2 σ) can also be used as an alternative way to evaluate TE materials, and increasing PF has been recognized as a key strategy in optimizing ZT, [8] particularly in the case of polymer-based TE materials where κ values are relatively low and similar in magnitude. TE materials with a higher PF value can convert more heat into electricity. One of the most pressing issues that researchers in this field are facing is the development of high-performance TE materials, which has proven to be difficult. Binary bulk chalcogenides such as bismuth telluride (Bi 2 Te 3) and antimony telluride (Sb 2 Te 3) are well-known to exhibit a maximum ZT value of more than 1.4 at room temperature, and are thus well-suited for near-room-temperature applications, such as refrigeration and waste heat recovery up to 200 °C. [10-12] However, using expensive inorganic TE modules to harvest thermal energy is