The friction coefficients of ionic liquids were evaluated by many investigations. Most investigations used fluorine-based ionic liquids as lubricants. However, these ionic liquids produce the corrosion wear. This investigation focuses on the use of cyano-based ionic liquids as lubricants. Compared to fluorine-based ionic liquids, cyano-based ionic liquids exhibit high friction coefficients against steel material. This work examines how the friction coefficients of cyano-based ionic liquids are influenced by the type of sliding material used (AISI 52100, TiO2, and tetrahedral amorphous carbon). TiO2 lubricated with 1-ethyl-3-methylimidazolium tricyanomethanide, and ta-C lubricated with 1-butyl-1methylpyrrolidinium tetracyanoborate exhibited very low friction coefficients, smaller than fluorine-based ionic liquids. Time-of-Flight Secondary Ion Mass Spectrometry analysis showed that anions adsorb onto the worn surface, suggesting that anion adsorption is a critical parameter influencing friction coefficients. Quadrupole Mass Spectrometry measurements revealed that cations decompose on the nascent surface, preventing adsorption on the worn surface. These results suggest that low friction coefficients require the decomposition of cations and adsorption of anions. The reactivity of nascent surface changes with the sliding material used due to varying catalytic activity of the nascent surfaces.