The tribological behavior of 316L stainless steel/CoCrMo alloy contacts under aqueous lubrication was investigated in this work. Three types of microgels including poly(N-isopropylacrylamide) (PNIPAM), polyacrylic acid (PAA), and poly(N-isopropylacrylamide-co-acrylic acid) (PNIPAM-co-PAA) were prepared and used as lubricant additives in aqueous solutions. Tribological tests were conducted using a ball-on-disk reciprocating tribometer, over a range of temperatures, pH, and concentrations of the microgels. The PNIPAM-co-PAA microgels were proven to have excellent anti-friction and anti-wear properties, depending on the temperature and pH values of the solutions. The maximum friction coefficient coincided with the lower critical solution temperature of the PNIPAM-co-PAA microgels at 32 °C. At the same time, the friction coefficient increased with the increase in pH value of the lubricant solution with the PNIPAM-co-PAA microgels. The unique thermal- and pH-sensitive properties of the PNIPAM-co-PAA microgels provided a new strategy for controlling the friction and wear of steel/CoCrMo alloy contacts under aqueous lubrication.