Testing was conducted on the bentonite portion of a Geosynthetic Clay Liner (GCL) for application to an environment characterized as having high concentrations of dissolved calcium ions. This environment presents conditions that might affect the long-term hydraulic function of the GCL as a component in a barrier system. Experiments were conducted to investigate first-exposure compatibility of a sodium bentonite GCL subject to the affects of acidic groundwater and second from the combined affects of acidic groundwater enriched with calcium. Relationships between the ionic exchange of sodium, potassium, magnesium and calcium species in the bentonite, and changes in hydraulic conductivity and electrical conductance are reported and discussed.