Bone diseases, for example, osteoporosis, cause excessive differentiation of osteoclasts and decreased bone formation, resulting in imbalance of bone remodeling and poor osseointegration, which can be considered a relative contraindication for titanium implants. Dopamine (DA) might provide a solution to this problem by inhibiting osteoclasts and promoting osteoblasts at different concentrations. However, current commercial implants cannot load bone-active molecules, such as DA. Therefore, this study aimed to develop a surface modification method for implants to achieve a controlled release of DA and enhance the resistance of titanium implants to bone resorption and bone regeneration. DA-loaded alginate-arginine-glycine-aspartic acid (RGD) (AlgR) coatings on a vaterite-modified titanium surface were successfully assembled, which continuously and steadily released DA. In vitro studies have shown that materials showing good biocompatibility can not only inhibit receptor activator of nuclear factor-kappa B (NFκB) ligand (RANKL)-induced osteoclastogenesis but also enhance the adhesion and osteogenic differentiation of human bone marrow mesenchymal stem cells (hBMSCs). The optimal DA-loaded concentration of this bidirectional regulation is 100 μM. Interestingly, DA more effectively attenuated osteoclastogenesis when released in a sustained manner from titanium coatings than it did via traditional, free administration, and the alginate-RGD coating and DA clearly exhibited great synergy. This study provides a design of titanium implant surface modification to improve bone remodeling around implants.