Abstract EPR investigations of thallium europium sulphate tetrahydrate (TEST) and thallium samarium sulphate tetrahydrate (TSST) single crystals, using Gd3+ probe ion, reveal that they undergo phase transitions similar to those reported in isostructural ammonium compounds, although the transition temperatures are consistently lower. This implies that the phase transitions are not associated directly with NH+ 4 molecular dynamics, although it does have an influence in shifting the transition temperatures.