problems in the process of their application. For example, the lubricating oils have leakage, climbing, and volatilization loss in the process of mechanical operation, which not only produce pollution and waste, but also cause lubrication failure. The use of grease can partially solve the leakage and climbing of lubricating oil, but itself also has some problems, such as poor lubrication performance due to introduction of thickener, poor cooling effect, and the high viscosity leading to the limited running speed of the mechanical bearing. It is exciting that the recently developed supramolecular gel lubricants are expected to solve these problems of lubricants and greases. [2] The gel lubricant looks like a semisolid grease, but it presents the characteristics of the lubricating oil due to the shear force and temperature rise making them turn into liquid in the sliding process. These characteristics can maintain good lubrication without affecting the speed of the mechanical and heat dissipation. At present, there are few reports on gel lubricants in the world. Mori and co-workers reported a thermally reversible gel lubricant, and found that the lubricating ability of the gel lubricant was related to the structure and concentration of the gelator. The tribological results show that the gel has a good lubrication performance mainly because the lubricant is easy to form an effective protective film on the contact surface. [3][4][5] Our group has designed and prepared a class of low molecular weight gelators that can gelate a variety of lubricating oils. [6][7][8][9] The experimental results show that the prepared new type of gel lubricant can effectively avoid the creep of lubricating oils and have better antifriction and antiwear properties than that of the lubricating oil and grease. [10] However, the above reported gel lubricants also have some defects, such as the complicated synthesis steps of the gelator, and the high cost of the raw materials. Therefore, designing and preparing highperformance, low-cost, and easy prepared gel lubricants is still one of the research hotspots in this field.In addition to the individual component geltors, a variety of two components can also form a complex by intermolecular noncovalent interaction, [11][12][13][14] and then gelate solvent to form a gel. For this complex, a single component in the solvent Here, reported is a new, simple, and nonsynthetic way of in situ preparation of bi-component supramolecular gel lubricants, which are formed by supramolecular self-assembly of bis(2-ethylhexyl) sulfosuccinate (AOT) and aromatic acid derivatives via the noncovalent interaction in the base lubricating oil. The formation mechanism of the gel lubricant was investigated by experimental and theoretical calculations. The results of 1 H nuclear magnetic resonance, ultraviolet, and molecular dynamics simulations show that they formed a network structure through intermolecular hydrogen bonding and π-π stacking, thereby solidifying the base oil to form gel. The rheological and thermal anal...