An in situ doping approach of producing Al-doped ZnO NWs was demonstrated using an aerosol-assisted chemical vapour deposition (AA-CVD) technique. In this technique, Zn precursor was kept in the middle of a horizontal tube furnace whereas the dopant solution was kept in an aerosol generator, which was located outside the furnace. The Al aerosol was flowed into the reactor during the growth of NWs in order to achieve in situ doping. Al-doped ZnO NWs were synthesized as verified by the combination of XRD, TEM/EDS and TOF-SIMS analysis. Highly (00.2) oriented ZnO seed layers were used to promote vertically aligned growth of Al-doped ZnO NWs. Lastly, a growth mechanism of vertically aligned Al-doped ZnO NWs was discussed.