Ionic liquids that melt slightly above room temperature (and may be called low-melting ionic solids, LMISs) were used as sensing materials for the detection of ions in aqueous solutions. A simple procedure based on the consecutive melting and further solidification of the LMISs was applied to prepare solid-contact ion-sensitive electrodes. A potentiometric response toward a number of anions was observed, and the possibility of altering the selectivity by incorporating additional ionophores into the LMIS matrix was demonstrated.