Applying hydrostatic pressure has emerged as a promising strategy for regulating the properties of thermoelectric materials, particularly in the case of β-CuSCN, which has garnered attention due to its ultra-low thermal conductivity and potential applications in thermoelectric devices. Herein, we investigate the intrinsic mechanism governing the electron-thermal transport properties of β-CuSCN under hydrostatic pressure. It was found that ZT decreased by 30 % along the in-plane direction while increasing by 24 % along the out-of-plane direction following the application of hydrostatic pressure, respectively. Our results reveal that the competitive relationship between pressure-driven effects on phonon dynamics and electronic structure influences the thermoelectric properties of β-CuSCN. For the transport mechanism, the compression alters phonon dispersion by enhancing atomic interactions, which leads to an increase in lattice thermal conductivity. On the other hand, despite strong coupling between electrical transport parameters, a net increase in power factor is achieved through pressure-induced bandgap narrowing. As a result, the thermoelectric properties demonstrate contrary variation tendency along the in-plane and out-of-plane directions. Our research deepens our understanding of transport behavior under extreme pressure conditions and provides valuable insights into the fundamental relationship between structural deformation and thermoelectric performance.
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