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Chalcogenide glass materials as membranes for potentiometric sensors for chemical analysis in solutions have been studied since more than 20 years. In this work, an electrolyte–insulator–semiconductor structure was combined with chalcogenide glass membranes prepared by means of the pulsed laser deposition technique. Depending on the membrane composition a selectivity to different ions (Cd2+ and Pb2+) is achieved. The different sensor membranes have been physically characterised using microscopy, ellipsometry, profilometry, atomic force microscopy (AFM), scanning electron microscopy (SEM) and Rutherford backscattering spectrometry (RBS). The electrochemical behaviour has been investigated via capacitance/voltage (C/V) and constant capacitance (ConCap) measurements and results in a Cd2+ sensitivity of 23.1 ± 0.6 mV per decade in a linear range from 7 × 10−6 to 10−2 mol/l and 24.4 ± 0.5 mV per decade in a linear range from 5 × 10−6 to 10−2 mol/l for Pb2+, respectively.