Carbon nanotubes (CNTs) with 10 nm average diameter and 5 μm in length were synthesized by electric arc discharge. The morphology and structure of CNTs were characterized by high resolution transmission electron microscopy (HRTEM) and X-ray powder diffraction. The tribological properties of CNTs as an additive on lithium grease were evaluated with a four ball tester. The results show that the grease with CNTs exhibit good performance in antiwear (AW) and decrease the wear scare diameter (WSD) about 63%, decrease friction reduction about 81.5%, and increase the extreme pressure (EP) properties and load carrying capacity about 52% with only 1% wt. of CNTs added to lithium grease. The action mechanism was estimated through analysis of the worn surface with a scanning electron microscope (SEM) and energy dispersive X-ray (EDX). The results indicate that a boundary film mainly composed of CNTs, Cr, iron oxide, and other organic compounds was formed on the worn surface during the friction process.