Polydopamine (PDA) prepared in the form of a layer of polymerized dopamine (DA) in a weak alkaline solution has been used as a versatile biomimetic surface modifier as well as a broadly used immobilizing macromolecule. This review mainly discusses the progress of biomaterial surface modification inspired by the participation of PDA in bone tissue engineering. A comparison between PDA-assisted coating techniques and traditional surface modification applied to bone tissue engineering is first presented. Secondly, the chemical composition and the underlying formation mechanism of PDA coating layer as a unique surface modifier are interpreted and discussed. Furthermore, several typical examples are provided to evidence the importance of PDA-assisted coating techniques in the construction of bone biosubstitutes and the improvement of material biocompatibility. Nowadays, the application of PDA as a superior surface modifier in multifunctional biomaterials is drawing tremendous interests in bone tissue scaffolds to promote the osteointegration for bone regeneration.