The Bi–Te thermoelectric system shows an excellent figure of merit (ZT) near room temperature. Research on increasing the ZT value for n‑type Bi–Te is imperative because the thermoelectric properties of this compound are inferior to those of the p-type material. For this purpose, n-type Bi2Te3-ySey powders with various amounts of Se dopant (0.3 ≤ y ≤ 0.6) were synthesized by a vacuum melting-grinding process to improve the physical properties. The ZT value of the sintered bodies was investigated in the temperature range of 298–423 K with regard to the electrical and thermal characteristics. As the Se content increased, the electrical conductivity decreased owing to a reduction in the carrier concentration, which improved the overall value of ZT. The thermal conductivity clearly decreased as the Se content increased in the temperature range of 298–373 K due to increased alloy scattering, as well as a reduction in the lattice thermal conductivity caused by crystal grain boundary scattering. At room temperature, Bi2Te2.7Se0.3 (y = 0.3) exhibited the highest ZT of 0.85. At increased temperatures, the ZT value was highest for Bi2Te2.55Se0.45 (y = 0.45), indicating that the optimal effect of the Se dopants varies depending on the temperature range.