Developing accurate self-assembly is the key for constructing functional materials from a bottom-up approach.At present,it is mainly hindered by building blocks and driving modes.We design a new self-assembly method based on the magnetic coupling between spin-polarized electrons.First-principles calculations show that spinpolarized electrons from different endohedral metallofullerene (EMF) superatoms can pair each other to ensure a one-dimensional extending morphology.Furthermore,without ligand passivation,the EMF superatoms maintain their electronic structures robustly in self-assembly owing to the core-shell structure and the atomic-like electron arrangement rule.Therefore,it should noted that the magnetic coupling of monomeric electron spin polarization can be an important driving mechanism for high-precision self-assembly.These results represent a new paradigm for self-assembly and offer fresh opportunities for functional material construction at the atomic level.