The synthesis was carried out via Z-selective Wittig and intramolecular homocoupling reactions with nickel complexes to yield decabutoxylated (25,25)MCNB (1) over 14 steps. NMR spectroscopy and DFTB-MD calculations revealed that the Möbius twist structure moves quickly around the molecule in solution. Photophysical measurements revealed that the synthesized MCNB exhibits greenish-blue fluorescence with a symmetry allowed S0→S1 transition caused by the lowered symmetry. Experimentally, chiral HPLC separation and CD spectroscopy revealed that the chirality originates from the Möbius topology. The combination of strain calculations with a rational synthetic strategy can be expected to create a variety of topological molecular nanocarbons, which will promote the progress of materials science in this area.