The response of borehole water levels to barometric pressure changes in semiconfined aquifers can be used to determine barometric response functions from which aquifer and confining layer properties can be obtained. Following earlier work on barometric response functions and aquifer confinement, we explore the barometric response function as a tool to improve the assessment of groundwater vulnerability in semiconfined aquifers, illustrated through records from two contrasting boreholes in the semiconfined Chalk Aquifer, East Yorkshire, UK. After removal of recharge and Earth tide influences on the water level signal, barometric response functions were estimated and aquifer and confining layer properties determined through an analytical model of borehole water level response to barometric pressure. A link between the thickness and vertical diffusivity of the confining layer determined from the barometric response function, and groundwater vulnerability is proposed. The amplitude spectrum for barometric pressure and instrument resolution favor determination of the barometric response function at frequencies to which confining layer diffusivities are most sensitive. Numerical modeling indicates that while the high frequency response reflects confining layer properties in the immediate vicinity of the borehole, the low frequency response reflects vertical, high diffusivity pathways though the confining layer some hundreds of meters distant. A characteristic time scale parameter, based on vertical diffusivities and thicknesses of the saturated and unsaturated confining layer, is introduced as a measure of semiconfined aquifer vulnerability. The study demonstrates that the barometric response function has potential as a tool for quantitative aquifer vulnerability assessment in semiconfined aquifers.