The article presents the synthesis and characterization of inter-[60]fullerene conjugates with inherent chirality. The authors describe a method to covalently link two open-[60]fullerenes, creating a double-caged structure with strong electronic communication and chiroptical activity. The conjugate exhibits a high dissymmetry factor of 0.21 at 674 nm, breaking the record for known chiral organic molecules. The synthesis involves a phosphine-mediated sequential deoxygenation reaction, which results in the formation of a fully conjugated, double-opened C20 nanocarbon with a well-defined structure. The electronic properties of the conjugate are explored through absorption spectra, electrochemical analysis, and theoretical calculations, revealing strong π-conjugation and intercage electronic communication. The chiroptical properties, including circular dichroism and dissymmetry factor, are also investigated, demonstrating the molecule's potential for applications in chiroptoelectronic devices.The article presents the synthesis and characterization of inter-[60]fullerene conjugates with inherent chirality. The authors describe a method to covalently link two open-[60]fullerenes, creating a double-caged structure with strong electronic communication and chiroptical activity. The conjugate exhibits a high dissymmetry factor of 0.21 at 674 nm, breaking the record for known chiral organic molecules. The synthesis involves a phosphine-mediated sequential deoxygenation reaction, which results in the formation of a fully conjugated, double-opened C20 nanocarbon with a well-defined structure. The electronic properties of the conjugate are explored through absorption spectra, electrochemical analysis, and theoretical calculations, revealing strong π-conjugation and intercage electronic communication. The chiroptical properties, including circular dichroism and dissymmetry factor, are also investigated, demonstrating the molecule's potential for applications in chiroptoelectronic devices.