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Bi2Te2.7Se0.3-based alloys are conventional n-type thermoelectric materials for solid-state cooling and heat harvest near room temperature; high thermoelectric performance over a wide temperature range and superior mechanical properties are essential for their use in practical thermoelectric devices. In this work, we demonstrated that decent thermoelectric performance can also be realized in an unconventional composite with a nominal composition of Bi2Te2.3Se0.7since the emergence of a Bi2Te2Se phase with Se ordered occupation could induce an enlargement of the electronic band gap. Follow-up Cu/Na codoping could generate a dynamic optimization of carrier concentration, significantly broadening the temperature range of high thermoelectric performance. Further B incorporation and annealing treatment resulted in obvious grain refinement and stacking fault structures, which help pushing the ultimate maximal figure of merit up to ∼1.3 at 423 K with an average value of ∼1.2 at 300–573 K. This work might provide insights for further research on bismuth tellurides and other thermoelectric materials.