Porous nanocrystalline Ln2Ti2O7 (Ln=Nd, Gd, Er) was prepared by a facile self-propagating combustion method using metal nitrates (Ln(NO3)3 (Ln=Nd, Gd, Er), TiO(NO3)2) and glycine. The photocatalytic activity of Ln2Ti2O7 (Ln=Nd, Gd, Er) was evaluated by the photocatalytic degradation of methyl orange (MO). The results showed that the photocatalytic activity of Ln2Ti2O7 (Ln=Gd, Er) with cubic pyrochlore structure was higher than that of Nd2Ti2O7 with monoclinic perovskite structure and Gd2Ti2O7 showed the best photocatalytic activity. The different photocatalytic activities observed for Ln2Ti2O7 (Ln=Nd, Gd, Er) could be related to its different crystal structures and Ln 4f shells.