The possibility of using mixed Fe2+/Fe3+ copper hexacyanoferrate (CuHCF) as the material for the transducer layer of solid-contact ion-selective electrodes (SC-ISEs) with plasticized polyvinylchloride membranes is studied. The study is performed for K+-SC-ISEs and water-hardness SC-ISEs. It is shown that CuHCF combines the ion-exchange and redox properties and, hence, in principle, should be suitable for SC-ISEs. However, the reproducibility of SC-ISE potentials from one electrode to another and their stability in time are far below those of conventional ISEs with internal aqueous solution. The potentials of individual SC-ISEs can be brought closer to one another by their polarization using a potentiostat or by their short-circuiting to a saturated silver-chloride reference electrode.