Bulk polycrystalline samples in the series Ti1-xNb x S2 (0≤ x ≤0.075) were prepared using mechanical alloying synthesis and spark plasma sintering. X-ray diffraction analysis coupled with high resolution transmission electron microscopy indicates the formation of trigonal TiS2 by high energy ball-milling. The as-synthesized particles consist of pseudo-ordered TiS2 domains of around 20-50nm, joined by bent atomic planes. This bottom-up approach leads, after spark plasma sintering, to homogeneous solid solutions, with a niobium solubility limit of x =0.075. Microstructural observations evidence the formation of small crystallites in the bulk compounds with a high density of stacking faults. The large grain boundary concentration coupled with the presence of planar defects, leads to a substantial decrease in the thermal conductivity to 1.8W/mK at 700K. This enables the figure of merit to reach ZT=0.3 at 700K for x =0.05, despite the lower electron mobility in mechanically alloyed samples due to small crystallite/grain size and structural defects.