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BACKGROUND: Inspired by natural bones, many organic components were added to Calcium Phosphate Cements (CPCs) to improve their mechanical strength. However, the strength of these composite CPCs is limited by the low strength of organic components itself and the weak interaction between organic components and CPCs. OBJECTIVE: Firstly, a composite CPC containing mussel-inspired adhesive, Poly-(Dopamine Methacrylamide-co-2-methoxy Ethylacrylate) (pDM) was developed. Secondly, the interactions between pDM and CPC and their effect on mechanical properties were investigated. METHODS: The interactions between pDM and CPC were performed by Nuclear Magnetic Resonance, Laser Raman, X-ray Photoelectron Spectroscopy, Fourier Transform-Infrared Spectroscopy and X-ray Diffraction Analysis. RESULTS: The toughness and compressive strength of pDM-CPC scaffold were both significantly enhanced, because of the enhanced interface binding strength among CPC and pDM due to their interaction and the improved mechanical strength of pDM owing to its self-oxidation cross-linking. The toughness of pDM-CPC scaffolds increased with the increased contents of pDM, while pDM-CPC scaffold containing 35 wt.% pDM had the highest compressive strength of all, which the latter was more than five times compared to that of CPC. CONCLUSION: The mechanically strong pDM-CPC scaffolds has potential application in bone regeneration as well as in craniofacial and orthopedic repair. [ABSTRACT FROM AUTHOR]