The on-surface self-assembly of inorganic atomic clusters and organic molecules offers significant opportunities to design novel hybrid materials with tailored functionalities. By adopting the advantages from both inorganic and organic components, the hybrid self-assembly molecules have shown great potential in future optoelectrical devices. Herein, we report the co-deposition of 4,8diethynylbenzo[1,2-d-4,5-d0]bisoxazole (DEBBA) and Se atoms to produce a motif-adjustable organic-inorganic hybrid selfassembly system via the non-covalent interactions. By controlling the coverage of Se atoms, various chiral molecular networks containing Se, Se 6 , Se 8 , and terminal alkynes evolved on the Ag(111) surface. In particular, with the highest coverage of Se atoms, phase segregation into alternating one-dimensional chains of non-covalently bonded Se 8 clusters and organic ligands has been noticed. The atom-coverage dependent evolution of self-assembly structures reflects the remarkable structural adaptability of Se clusters as building blocks based on the spontaneous resize to reach the maximum non-covalent interactions. This work has significantly extended the possibilities of flexible control in self-assembly nanostructures to enable more potential functions for broad applications.