(R)-3a) were obtained in the reaction though with relatively inferior enantioselectivities while using the trans N-tosylhydrazones 2. These results indicated that both cis and trans substrates exhibited good compatibility in the asymmetric carbene cross-coupling reaction and featured a stereospecific manner. In addition, N-tosylhydrazones substrates bearing the 3-monosubstited amide moieties, including the diisopropyl, dipropyl, dicyclohexyl and methyl tert-butyl groups, were all favorable in this coupling reaction under condition A, thus producing the desired products ((S)-4g-4j) in 80%-92% yields with 82-88% ee values. The ester group (CO2Ad) substituted product (R)-4k could be achieved as well in 90% yield with 80% ee starting from the trans hydrazone substrate. When we selected trans-2n as the substrate under condition A, the corresponding product (R)-3a was obtained in a severely decreased yield (49%) and relatively lower ee value (78% ee) as a comparison to the case of (S)-3a from cis-2a, which is 95% yield with 91% ee in scheme 2. without any loss of enantiopurity, which are ubiquitous in biomolecules and pharmaceuticals. Additionally, 1,2-amino alcohols (5f, 5g) could be synthesized through the nucleophilic attack of free amine to epoxides. Reduction of the axially chiral amide (S)-4a worked well enabled by LiAlH4, thus affording the tertiary amine 5h in 97% yield. These results fully indicate that 3-substituted axially chiral cyclobutylidenes can serve as valuable building blocks, offering a promising blueprint for the synthesis of bioactiverelated compounds.