Based on the first principles and wave function analysis theory,the one?photon absorption (OPA) spectra and two?photon absorption (TPA) spectra of the zigzag boundaries Twisted Bilayer Graphene Nanosheets (Z?TwBLG?NS) with different twist angles and their electronic excitation characteristics were studied.Firstly,the law and properties of the change of one?photon absorption spectrum and two?photon absorption spectrum with different twist angle were studied.Secondly,the characteristics of electron transition were analyzed visually.The results show that the absorption peaks are red?shifted to different degrees when the angle is not 0°,indicating that the angle modulates the absorption spectra of the system.The Z?TwBLG?NS with an angle of no 0° had obvious boundary effect, and the isosurface of electrons and holes were mainly distributed at the edge. Finally,the limiting effect of moiré pattern on electron transfer was revealed,which was reflected in the difference in the density of electrons and holes gathered in the moiré pattern.This study provides the analytical basis of physical mechanism for the generation of optical properties of Z?TwBLG?NS under the control of twist angle,as well as a research methodology for related research work.