In this work we present a simple method to synthesize nanostructured, bismuth-doped lead telluride by co-ball-milling. The obtained nanopowders were compacted via either a cold pressing/annealing approach or by hot pressing. The two compacting methods were compared regarding sample density. Series with bismuth content up to 6 at.% were characterized by measuring the thermoelectric transport properties over a wide temperature range between 123 K and 773 K using two different techniques for the Seebeck coefficient and electrical conductivity. A decreasing thermal conductivity and increasing electrical conductivity were found with increasing doping level. The best results were obtained for samples with 5 at.% and 6 at.% bismuth, showing a maximum ZT value of 1.1 at 773 K. Transmission electron microscopy study was performed to analyze the microstructure of the nanopowders, suggesting that, in addition to n-type doping of the lead telluride matrix, segregation effects occur and the samples consist of multiple phases.