Objective: The aim was to prepare a new calcium-decorated titanium surface and investigate whether this new modified titanium surface could enhance bone formation and osseointegration. Materials and methods: In this study, we prepared a calcium-decorated titanium (Ti) surface through hydrothermal treatment with a mixed solution of phytic acid (PA) and calcium hydroxide [Ca (OH)(2)]. Pure titanium with a sandblasted/acid-etched (SLA) surface was used as the control group. The physical properties of different titanium surfaces such as the surface morphology, elemental composition, wettability, and surface roughness were investigated. The effect of biomineralization was studied by soaking samples in simulated body fluid (SBF). The cell adhesion, proliferation, and osteogenic differentiation of human bone marrow mesenchymal stem cells (hBMSCs) were evaluated as well. Results: Calcium-decorated titanium surfaces with superior hydrophilicity were successfully prepared. X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDX) confirmed that the calcium ions were decorated onto the titanium surface and were continuously released with time. After immersion in 10SBF for 1 day, a hydroxyapatite layer formed on both modified surfaces. In vitro tests showed that the modified surface enhanced the cell adhesion, proliferation, and osteogenic differentiation of hBMSCs. The expression levels of the osteogenic-related genes were significantly upregulated compared to the control samples. Conclusions: The calcium-decorated titanium surface enhanced the bioactivity and osteogenesis ability of the titanium surface, which suggests that calcium-decorated materials would have great potential for not only dental implants but also various other biomaterial applications.