We refine the crystal structures of a systematic series of compounds with the general composition Ho(x)Yb(2-x)TiO5 (x = 2, 1.6, 1.2, 1, 0.8, 0.4, 0) and Er2TiO5 and find a transition from defect-pyrochlore to defect-fluorite structure with increasing ytterbium content, decreasing lanthanide radius. Short-range structure modulations consisting of pyrochlore-like nano-domains are systematically characterised using transmission electron microscopy. We test the Kr2+ 1 MeV ion-irradiation response of Ho2TiO5, HoYbTiO5, Yb2TiO5, and Er2TiO5, via the crystalline to amorphous transition observed by using the in-situ TEM approach. The critical dose of amorphisation, D-c, was measured at various temperatures and used to calculate the critical temperature for maintaining crystallinity, T-c. A trend of lower T-c values with decreasing lanthanide radius is found. We describe a new approach for determining T-c values using cross-sectional TEM analysis of ex-situ bulk irradiated, 1 MeV Se+, samples; Ho2TiO5, HoYbTiO5 and Yb2TiO5. The results of D-c and T-c values using the two approaches vary; however the trends across the sample system remain the same. Crown Copyright (C) 2018 Published by Elsevier B.V. All rights reserved.