The bioinspired material 3,4-dihydroxy-L-phenylalanine (DOPA) is commonly used as a basic layer in surface modification for osteogenesis; however, its effects on bone remodeling and the underlying mechanisms remain unclear. Here, we investigated the effect of DOPA-coated surfaces on human bone marrow-derived mesenchymal stem cells in vitro. Cells cultured on DOPA-modified titanium discs exhibited enhanced cellular adhesion and spreading compared with cells on non-treated surfaces. Moreover, DOPA-coating promoted greater cell proliferation and osteogenic differentiation, as determined using cell counting kit-8 (CCK-8) assay, alkaline phosphatase activity test and quantitative mineralization measurements. Furthermore, microarray analysis revealed that genes participating in focal adhesion were upregulated on DOPA-coated surfaces. Our results indicate that the application of a simple DOPA coating can promote osteogenic differentiation of osteoprogenitor cells, improving new bone formation and bone remodeling around implantable devices in tissue engineering.