Bone remolding involves the formation of new bone by osteoblasts and the absorption of old bones by osteoclasts. Due to the vital role of osteoblasts and osteoclasts during bone regeneration, it might be feasible to promote osseointegration around the titanium implants by stimulating osteoblasts and inhibiting osteoclasts by modifying the surfaces of the implants. Lithium is used in the treatment of psychiatric patients, and it may be associated with osteogenesis. In this study, lithium was incorporated with sandblasted, large-grit and acid-etched titanium implants via a hydrothermal treatment. In vitro, the nano-scale surface enhanced the adhesion and proliferation of bone marrow mesenchymal stem cells (BMSCs). Moreover, the SLA-Li surface displayed a negative effect on the process of osteoclastogenesis. Further mechanism analysis indicated that the canonical Wnt/β-catenin signaling pathway was activated according to the results of RT-PCR and western blotting. More importantly, the RANKL/OPG signaling axis was also involved in these effects on the SLA-Li surface. The experiments in vivo proved that the SLA-Li surface could induce the bone formation and osseointegration during the early osseointegration after the dental implant surgery. These results suggested that bone homeostasis could be manipulated by an SLA-Li surface, which implied that this new surface might serve as a promising material for clinical application in the future.