Bulk samples of six Ln2TiO5 compounds with Ln = La, Pr, Nd, Eu, Gd and Tb were prepared and characterised. Most of the samples have a phase purity of ∼95% (based on BEI and EDS) with the predominant secondary phase primarily being Ln2Ti2O7. Using XRD, TEM selected area diffraction and high resolution imaging techniques, we have confirmed the results of previous studies which showed that at room temperature Pr2TiO5, Nd2TiO5, Eu2TiO5 and Tb2TiO5 have orthorhombic structures with Pnma symmetry. The structure of Tb2TiO5 was further monitored as a function of temperature. The relevance of Ln2TiO5 compounds to advanced nuclear fuel cycles is discussed.