Nanomaterials exhibit intriguing tribological performance and have received particular attention in the lubrication field. However, little research has been found that surveyed the application of nanometer Ni in lithium grease. In this study, nanometer Ni with an average size of 100 nm was synthesized by the direct reduction method and dispersed in lithium grease. The feasibility of nanometer Ni as a grease additive in different lubrication scenarios was evaluated by a four-ball friction tester and a TE77 reciprocating friction tester. The lubrication mechanism was analyzed based on the evaluated physical properties of lithium grease and the characterization of the wear surface. The tribology test results showed the tribological properties of lithium grease were enhanced after introducing nanometer Ni. When the dosage was 0.2 wt%, the friction-reducing and anti-wear properties of point-to-point contact increased by 34.8% and 35.2%, respectively, while those of the point-to-flat contact increased by 28.8% and 38.7%, respectively. Our work not only provides theoretical guidance and practical reference for the utilization of nanometer Ni in grease, but also explains several possible lubrication mechanisms of nanomaterials in grease.