The emerging fields of the Internet of Things, intelligent robotics, and smart biomedical devices have sparked an increasing demand for high-performance thermoelectric (TE) devices due to their efficient conversion of thermal energy into electrical power, and vice versa. The environmentally friendly (Bi, Sb)2Te3 (BST) system, which displays superior performance near room temperature, offers a promising solution for optimizing thermoelectrics to meet the needs of commercial applications. Here, we utilized AgInSe2 alloying to enhance the TE and mechanical properties of BST, aiming to optimize electron and phonon transport and elucidate the underlying mechanisms. The synergistic optimization resulted in a peak zT of ∼ 1.3 at 353 K and an average zTave of ∼ 1.11 from 303 K to 503 K in BST-0.1 %AgInSe2, as well as a high Vickers hardness of ∼ 105 Hv. Through rational optimization of the TE device, we achieved a maximum conversion efficiency of ∼ 6 % at a temperature difference of 210 K. Leveraging the robust TE output of the device, we further evaluated its potential as a self-powered information interaction wristband device based on ASCII codes. We envisage this versatile TE device being extensively applied in power generation and human–machine interaction, with promising potential in wearable electronics, telecommunications, and healthcare monitoring.