Clay buffer is a key component of the engineered barrier system (EBS) for geological disposal of higher activity radioactive waste. Experimental observations indicate the possibility of buffer erosion at the interface with host rock due to interactions with groundwater. Existing models for clay erosion are very limited in terms of addressing the hydro-chemical effects, while the assessment of the long-term performance of clay buffer requires robust predictive models covering expected environment conditions and multiphysics phenomena involved in the erosion process. The work presented here is a step towards such a predictive capability, which considers clay expansion, detachment of clay particles and transport of detached particles by groundwater within a single modelling framework. The effects of solution chemistry and flowrate on the penetration, extruded mass and particle release rate of clay buffer are investigated in this paper. A series of experimental data are used to validate the swelling and erosion model developed in this study. The results show that the extrusion distance, which is controlled by both clay swelling and detachment processes, is nearly linearly dependent on the water flowrate irrespective of the water chemistry. Similar linear dependence of the erosion rate on water flowrate is observed for flowrates less than 10−5 m/s. Higher water flowrates are shown to induce nonlinearly increasing erosion rates in accordance with experiments. A flowrate threshold is found above which the erosion behaviour of compacted bentonite can be significantly affected. A concept of tolerance time for clay buffer is introduced as a failure criterion. The results indicate that the coupled effect of water chemistry and velocity requires further investigation for ionic concentrations below 1 mM.