In this study, n-type Cu and Zn metal nanoparticle decorated Bi₂(Te₀.₉Se₀.₁)₃ ingots were prepared by a large-scale zone melting technique, with the concept of 'nanoparticle-in-alloy' to separately tune the electrical and thermal transport properties. Cu and Zn additions play multiple but different roles in the materials, whereas both of them form metal nanoinclusions embedded in van der Waals gaps or grain boundaries, exerting influences on thermoelectric properties. Cu addition, accommodated in the tetrahedral vacancies formed by four Te(1) atoms, effectively adjusts the electron concentration by donating its valence electron, and appreciably optimizes the power factor. Coupled with the significant frustration of heat-carrying phonons by Cu nanoinclusions, a highest ZT of 1.15 can be achieved for the 1 at.% Cu sample, which is an ∼20% improvement compared with that of commercial halogen-doped ingots. Zn addition, however, acting as weak donor, noticeably increases the density of state effective mass and Seebeck coefficient, and gives rise to a high ZT of 1.1. In particular, the kilogram-grade production technique coupled with the high ZT makes metal nanoparticle decorated n-type materials very promising for commercial applications.