Synthesis and tribological evaluation of three tetraalkylammonium thiomolybdate (R 4 N) 2 MoS 4 (R = methyl, propyl, or ammonia) aqueous-based lubricant additives on a ball-on-disk tribometer was carried out for a steel-aluminum contact. Tests were performed at the same conditions of load, entrainment speed, sliding distance, temperature, and concentration of MoS 2 to compare the activity (lubrication effect) of the thiomolybdates prepared. A friction reduction is observed for the three salts compared to pure water; however, significant differences in friction coefficient are observed depending on the alkyl group. SEM/EDAX and Raman analysis of the wear tracks reveal the in-contact formation of a MoS 2 -lubricating film, rich in molybdenum and sulfur.Lubricant additives, such as friction modifiers and mild antiwear agents, are added to lubricants for the purpose of minimizing surface asperity contact that may occur in a given machine element. Dichalcogenides (i.e., graphite, molybdenum disulfide), esters, and fatty acids are representative additives typically used for these purposes. Their molecules have a polar head and a lubricant-soluble tail, and when an additive-containing lubricant enters into the contact, the polar head anchors on metal surfaces forming a low-shear tribological film that prevents surface asperity contact and facilitates sliding motion [1]. As long as the mechanical contact is not heavily loaded, these molecules provide a cushioning effect that reduces surface interactions and thus reduce friction. However, as load and metallic contact increase, the strength of the additive and the chemical reaction process must increase. This leads to the use of sulfur-phosphorus-based EP additives, which form organometallic salts on the loaded surfaces that serve as sacrificial films to protect against aggressive surface damage. Frictional heating on continuously modified surfaces boosts chemical reactions and interactions between lubricating additives and the corresponding surfaces in the contact zone. Characteristics of the lubricating films formed in the contact depend on tribological mating pairs, chemical nature of the additive, and operating conditions.Considerable asperity contact is present in the boundary lubrication regime where the contacting surfaces are no longer separated by the lubricant. Under these conditions, friction characteristics of the mating pairs are entirely determined by the properties of the solids, and any lubricating film formed at the interface and the friction coefficient is essentially independent of fluid viscosity. The average film thickness formed in this regime is thinner than