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SrFBiS2 is a quaternary n-type semiconductor with rock-salt-type BiS2 and fluorite-type SrF layers alternately stacked along the c axis. The tunability of the crystal and electronic structures as well as the intrinsically low thermal conductivity make this compound a promising parent material for thermoelectric applications. In the current work, we show that alloying of Se and S in SrFBiS2 reduces the optical band gap with the second conduction band serving as an electron-transport medium, simultaneously increasing the electron concentration and effective mass. In addition, the raw material Bi2Se3 is shown to act as liquid adjuvant during the annealing process, favoring preferred-orientation grain growth and forming strengthen microstructural texturing in bulk samples after hot-pressed sintering. Highly ordered lamellar grains are stacked perpendicular to the pressure direction, leading to enhanced mobility along this direction. The synthetic effect results in a maximum power factor of 5.58 μW cm−1 K−2 at 523 K for SrFBiSSe and a peak zT = 0.34 at 773 K, enhancements of 180% compared with those of pristine SrFBiS2.