A new type of solid-contact ion-selective electrode (SC-ISE) has been developed that uses colloid-imprinted mesoporous (CIM) carbon with 24 nm diameter, interconnected mesopores as the intermediate layer between a gold electrode and an ionophore-doped ISE membrane. For a demonstration, valinomycin was used as K+ ionophore, and a good Nernstian response with a slope of 59.5 mV/decade in the range from 10-5.2 to 10-1.0 M was observed. The high purity, low content of redox-active surface functional groups and intrinsic hydrophobic characteristics of CIM carbon prepared from mesophase pitch lead to outstanding performance of these sensors, with excellent resistance to the formation of a water layer and no interference caused by light, O2, and CO2. When a redox couple is introduced as an internal reference species, calibration-free SC-ISEs can be made with a standard deviation of E° as low as 0.7 mV. Moreover, the interconnected mesopore structure of ISE membrane-infused CIM carbon facilitates both ion and electron conduction and provides a large interfacial area with good ion-to-electron transduction. Because of the large double layer capacitance of CIM carbon, CIM carbon-based SC-ISEs exhibit excellent potential stability, as shown by chronopotentiometry and continuous potentiometric measurements. The capacitance of these electrodes as determined by chronopotentiometry is 1.0 mF, and the emf drift over 70 h is as low as 1.3 μV/h, making these electrodes the most stable SC-ISEs reported so far.