In summary, an all sp 2 -hybridized, triply twisted Möbius carbon nanobelt (1) with a doublestranded structure was synthesized and isolated in single-crystal form. The success relies on: (i) proper choice of the precursors with saturated -CH2-CH2-bonds and preferable bond angles, (ii) efficient macrocyclization by Suzuki coupling reaction to form a triply twisted, pre-organized intermediate with a minimal strain, (iii) regio-selective Bi(OTf)3-catalyzed cyclization reaction of vinyl ethers for benzannulation, and (iv) aromaticity-driven oxidative dehydrogenation at last step to generate the final fully conjugated MCNB with large strain. Based on the experimental and theoretical calculations, 1 has a dominant localized aromatic character. The chiral resolution of 2b and 1 were successfully achieved, where 1 demonstrated a large absorption dissymmetry factor (|gabs| = 0.019) for the S0→S1 transition due to its D3 symmetry, efficient π-conjugation along the skeleton, and favorable alignment of the electric and magnetic transition moments. The synthetic strategy developed in this work could promote the synthesis of diverse topological molecular carbons with persistent chirality in the future.