“…Ionic liquids (ILs) are molten salts known to comprise cations and anions and constitute a fascinating class of solvents that has attracted the scientific community for decades due to the singularity of their physicochemical properties. − For their wide applications in green chemistry ranging from catalysis, − reaction, − separation, − and electrochemistry, the interface plays an essential and ubiquitous role, which has been the focus of IL research in the past 10 years. The competition, coexistence, and cooperation of interactions between ions and ion–substrate in interfacial ILs have been a breeding ground for novel properties and applications of ILs. ,, Controllable manipulation of various interactions via, for example, exposure to temperature and electric fields could lead to a new device paradigm for future chemical engineering. − …”