Bone endoprosthesis in patients with systemic chronic inflammation frequently leads to poor osseointegration after implantation mainly due to the increase in pro-inflammatory cytokines that induce bone resorption and impair bone formation. In this work, peptide-coated implants are designed to create a beneficial bone immune microenvironment around prostheses to promote interfacial osteogenesis. By taking advantage of the spontaneous and stable coordination chemistry, Ti-based implants are coated with the mussel-inspired peptide to mitigate lipopolysaccharide (LPS)-induced inflammation by up-regulating the M2 phenotype of macrophages. In addition, the peptide coating increases the bone-implant contact (BIC) by nearly 3 times resulting in suppressed osteoclastogenesis and promoted osteogenesis by inhibiting the nuclear factor kappa-B (NF-κB) signalling pathway. Our findings indicate that biomimetic peptides with osteoimmunomodulatory bioactivity can be incorporated into Ti-based prostheses to facilitate bone regeneration in patients with chronic inflammatory diseases.