Topological molecular carbons such as twisted and knotted carbon nanostructures are attracting increasing attention not only because they are aesthetically beautiful, but also due to their promising applications for electronics, photonics and spintronics. Among them, Möbius striplike molecules with an odd number of twists are of particularly interest (Fig. ) because they are topologically chiral, and they can serve as model compounds to validate the theoretically predicted [4n] Möbius aromaticity. Synthesis of this type of molecules is extremely challenging as one needs to carefully control both structural flexibility and large strain induced by the twist. The first non-conjugated Möbius molecule was synthesized by Walba et al in 1982 via a macroetherification reaction, while the first π-conjugated all-hydrocarbon Möbius molecule was reported by Herges and co-workers in 2003, which also demonstrated weak Möbius aromaticity. Later on, Latos-Grażyński and Osuka's teams independently discovered Möbius aromaticity and antiaromaticity in expanded porphyrinoids. The last decade has witnessed a rapid growth of a family of topological molecular carbons, the cyclo-para-phenylenes (CPPs), which are also called as "carbon nanohoops". The synthetic methods developed by Jast, Itami, Yamago and Isobe et al nicely solved the long-standing problem arisen from the large strain in the final CCP rings. Inspired by these progresses, chemists are now moving on to synthesize even more challenging carbon nanostructures such as twisted and knotted molecules containing fully conjugated units. For example, a number of CPP-based Möbius strip-like or mechanically interlocked molecules have been reported. These structures mainly contain single-stranded CPP rings and thus the π-conjugation is limited due to the significant tortional angles between the 1,4-phenylene units. Therefore, double-stranded, fully π-conjugated Möbius nanobelts become new targets. In 2019, Tanaka and coworkers reported the efficient synthesis of a CPP-based Möbius belt with a single twist and double strands by employing rhodium-catalyzed alkyne cyclotrimerization (Fig. ). Later, in 2021, Zhu and co-workers reported a sulfur-embedded, double-stranded Möbiusshaped belt (Fig. ) mainly by using Ullmann-type couplings followed by intramolecular Friedel-Crafts reactions. However, these two double-stranded Möbius molecules are not fully conjugated because their backbones are linked partially by either saturated (-CH2O-) or sulfur atom (-S-) linkers. Finally, in 2022, Itami, Segawa, and their co-workers reported the synthesis of the first singly twisted, double-stranded, all-sp 2 Möbius carbon nanobelt (MCNB) over 14 steps via Z-selective Wittig reactions followed by nickel-mediated intramolecular homocoupling reactions (Fig. ). The successfully isolated (25,25)MCNB was calculated to have a strain energy of about 49.4 kcal/mol, while the attempted synthesis of smaller-size MCNBs failed due to their larger strain. Different from the singly twisted Möbius structures, the Möbius systems with higher twists (e.g., the triply and quintuply twisted) (Fig. ) could have smaller strain energy per each twist and thus synthetically it may be more accessible from the viewpoint of strain energy. On the other hand, it requires more careful control on the conformation at each twist due to the structural flexibility. So far, only two π-conjugated, triply twisted Möbius molecules have been reported by Herges, Durola, and their co-workers (Fig. ). Again, due to their single-stranded structure, the cyclic π-conjugation is limited. Therefore, a highly twisted MCNB with a fully conjugated double-stranded structure remains exclusive. Herein, we report the facile synthesis of the first triply twisted MCNB (1, Fig. ) by rational design, and its chiral resolution which gave two enantiomers showing promising chiroptical properties.