Thermoelectric material Bil-xSbx nanowire arrays have been successfully synthesized by pulsed electrochemical deposition from aqueous solutions into porous anodic alumina membranes. X-ray diffraction results show that the as-synthesized nanowires are single-crystalline and have a highly preferential orientation. Scanning electron microscopy and transmission electron microscopy observations indicate that the ordered Bil-xSbx nanowire arrays are high filling and the diameters of the nanowires are modulated by the pulsed time. Energy dispersive spectrometer analysis indicates that the composition of the nanowires can be tuned by changing the solution concentrations.