A mixture of elemental Cr-Si powders has been subjected to mechanical alloying (MA) at room temperature to prepare CrSi2 thermoelectric compound.The MA powders were sintered at 800-1000 °C Cunder 60 MPa using spark plasma sintering (SPS) technique. Due to the observed larger loss of Si relative Cr during ball milling, the starting composition was modified to Cr30Si70, Cr31.5Si68.5 and Cr33Si67 to get a single phase of CrSi2 compound. The single phase CrSi2 has been obtained by MA of Cr31.5Si68.5 mixture powders for 70 h and subsequently sintered at 1000 °C. X-ray diffraction data shows that the SPS compact sintered at 1000 °C consists of only nanocrystalline CrSi2 compound with a grain size of 250 nm. The value of Seebeck coefficient of CrSi2 compound increases with temperature and reaches maximum value of 245 µV/K at 300 °C.