In this work, we theoretically investigate the linear and nonlinear optical absorption properties of open triangulene spin chains and cyclic triangulene spin chains in relation to their lengths and shapes. The physical mechanism of local excitation within the triangular alkene unit and the weak charge transfer between the units are discussed. The uniformly distributed electrostatic potential allows the system to have a small permanent dipole moment that blocks the electronic transition in the light excitation such that the electronic transition can only be carried out between adjacent carbon atoms. The one-photon absorption (OPA) spectra and two-photon absorption (TPA) spectra are red-shifted with the addition of triangulene units compared to N = 3TSCs (triangulene spin chains, TSCs). Here, TPA is mainly caused by the first step of the transition. The length of the spin chain has a significant adjustment effect on the photon cross-section. TSCs of different lengths and shapes can control chirality by adjusting the distribution of the electric dipole moment and transition magnetic dipole moment. These analyses reveal the photophysical properties of triangulene and provide a theoretical basis for studying the photophysical properties of triangulene and its derivatives.