Thermoelectric materials convert heat flux to electricity (or vice versa as Peltier coolers); however, their application to harvest waste heat is limited by challenges in fabrication and materials optimization. Here, cold-spray deposition is used as an additive manufacturing technique to fabricate p- and n-type Bi2Te3, on substrates ranging from quartz to aluminum.The sprayed material has a randomly oriented microstructure largely free from pores (> 99.5% dense), and deposition is achieved without substantial compositional changes. The Seebeck coefficient and thermal conductivity are largely preserved through the spray process, but the defects introduced during deposition significantly increase electrical resistivity. Defects can be removed, and compressive strain relaxed by a post-deposition anneal, which leads to Bi2Te3 blocks with a typical ZT of 0.3 at 100°C. Generators fabricated on sheets or pipes made of copper compare favorably with similar designs constructed using bulk Bi2Te3, displaying a wider operating temperature range. These results demonstrate the power and versatility of cold-spray additive manufacturing and provide a pathway toward fabrication of thermoelectric generators in complex geometries that are inaccessible to generators made by traditional approaches.