With the aim of improving the tribological properties of low-viscosity gear oil for automobiles, an acrylate of dialkyl dithiophosphoric acid (ADDP) with strong polar groups was synthesized. The tribological behavior of ADDP combined with molybdenum dialkyl dithiocarbamate (MoDTC) in gear oil was systematically studied. Tribological performances of gear oil containing different additives were assessed using a four-ball friction and wear tester. The obtained tribological characteristics reveal that ADDP and MoDTC can significantly improve the antiwear and antifriction performance of low-viscosity gear oil. Moreover, compared with using MoDTC or ADDP alone, the average friction coefficient and wear scar diameter of ADDP combined with MoDTC further decreased by 2.41–19.15% and 5.00–18.19%, respectively. Analysis of the worn surface showed that the structural characteristics and physical synergistic lubricating actions of the ADDP with MoDTC additives during the friction process can contribute to the exceptional tribological properties of the hybrid additives.