Ultrasmall CuCo2S4 nanocrystals (NCs) have been demonstrated as an effective agent in the photothermal therapy (PTT) of tumors, but have not been investigated for treatment of arterial inflammation, which is critical in the initiation and development of atherosclerosis (AS), a leading cause of vascular diseases worldwide. In this study, CuCo2S4 NCs were synthesized and used as an efficient PTT nanoplatform for arterial inflammation. In vitro experiments illustrated an effective ablation of inflammatory macrophages by CuCo2S4 incubation combined with the irradiation with an 808 nm near-infrared (NIR) laser. In vivo experiments in an apolipoprotein E knockout (Apo E-/-) mouse model showed that the local injection with CuCo2S4 followed by irradiation with an 808 nm NIR laser notably ablated infiltrating inflammatory macrophages and effectively reduced arterial inflammation and arterial stenosis. This work provides a new strategy for treatment of AS by exploring bimetal sulfides as effective PTT agents.