Metatitanic acid was adopted as the raw material to prepare Fe-doped TiO2 nanocrystalline composite particles using suspension polymerization and sol-gel method, which were then characterized with XRD, TEM, TG-DTA and IR, etc.. The results showed the samples were nanocrystal accumulated porous particles, with average particle size of 29nm. Through doping of Fe3+ ion, the photo catalytic activities of particles under Xe lamp were investigated by photodegrading the methyl orange. It was found that, the TiO2 nanocrystal doped with 0.5% Fe3+ ion (accounted as mass fraction) had the highest catalytic activity. The Fe-doped TiO2 nanocrystalline composite particles prepared in this study has high activity, is easy for separation, recovery and reuse.