Recently, much attention has been focused on the design and synthesis of molecules with aromatic Möbius topology. One of the most promising applications is the manufacture of Hückel-to-Möbius topological optical switches with high nonlinear optical properties. In this work, we evaluate the electronic and vibrational contributions to static and dynamic nonlinear optical properties of the CS Hückel and C2 Möbius topologies synthesized by Herges and co-workers (Ajami, D. et al. Nature2003, 426, 819). Calculations are performed at the HF, B3LYP, BHandHLYP, BMK, M052X, CAM-B3LYP, and MP2 levels with the 6-31+G(d) basis set. Our results conclude that the BHandHLYP, M052X, and CAM-B3LYP methods correctly reproduce the X-ray crystal structure and provide similar nonlinear optical properties.