AimsTo investigate the biomimetic fabrication of fibrous-like organic-inorganic hybrid structures via a simple bottom-up approach, viz. self-assembly of simple molecules, and apply fibrous-like composites as a novel primer to improve dentin bond strengths of self-etch adhesives. Materials and methodsThe resultants of commercial amorphous calcium phosphate (ACP) nanoparticles and 10-methacryloyloxydecyl dihydrogen phosphate (MDP) ethanol-aqueous solution were analyzed by TEM, SEM, XRD, DLS and AFM. The acid and alkali resistance of abovementioned self-assembled composites were analyzed with TEM. Micro-tensile bond strengths (MTBS) tests were performed after polished dentin surfaces were pretreated with self-assembled composites. The pretreated dentin surfaces and dentin-resin interfaces were characterized by SEM/TEM. Key findingsACP nanoparticles in MDP solution could self-assemble into fibrous-like nanotube structures in 8 nm diameter. Self-assembly and self-proliferation process went from ACP nanoparticles, dissolved ACP nanoparticles (less than 50 nm), twig-like structures and fibrous-like nanotubes to cellular networks. The fibrous-like nanotubes were only detected when the amount of ACP in reaction system were more than 0.01 g. The more ACP interacted with MDP, the more fibrous-like nanotubes were formed. After the dentin surfaces were treated with fibrous-like nanotube composites, MTBS could be significantly improved. Moreover, the fibrous-like nanotube structures could be resistant to acidic challenge, and were stable at least for 3 months. SignificanceThe fibrous-like nanotube structures could be self-assembled via a bottom-up approach at certain ratio of MDP and commercial ACP nanoparticles. The application of fibrous-like nanotube composites as a novel primer prior to self-etch adhesives greatly improved dentin bond strengths.