This study investigates the possibility of modifying lubricating greases by 2D graphene oxide (GO) and lithium iron phosphate (LiFePO4) to enhance their tribological performance. GO's layered structure plays a crucial role in reducing friction by facilitating easy sliding between rubbing surfaces, making it an effective solid lubricant. The impact of these additives on friction reduction, wear resistance, and the tribolayer formation ability is evaluated by ball‐on‐disc tribometry with an emphasis on durability and sustainability. Comparative results reveal that unmodified greases exhibit a high susceptibility to wear, including oxide formation and severe plastic deformation. In contrast, greases with GO show a notable reduction in friction, while the addition of LiFePO4 contributes to the formation of a continuous protective layer that substantially reduces abrasive wear. The combination of GO and LiFePO4 results in a homogeneous, durable tribofilm that effectively protects surfaces against severe wear providing long‐term friction stability. Although lab‐scale LiFePO4 is used, the findings suggest a great potential for extending the useful life of recycled LiFePO4 from lithium‐ion batteries, similar to commercial LiFePO4 thus confirming significant improvements in the grease performance but also highlighting the potential to advance toward more sustainable solutions in industrial applications and electric vehicles.