Frontier molecular orbitals, i.e., HOMO and LUMO levels, along with HOMO-LUMO gap (E g ), are critical properties in evaluating the electronic and optical properties, electric conductivity, charge transport, and chemical reactivity of materials. Specifically, understanding the distribution of these fundamental properties across various sizes of fullerenes is essential for designing and optimizing fullerenes and their derivatives with specific requirements, such as improved conductivity, enhanced light absorption, or more favourable reactivity. In contrast to the distribution of E b values, the distribution of E g exhibits a lower dependence on the size of the fullerene cage, as showed in Figure and Figure ). The distributions of HOMO and LUMO also exhibit weak dependence on the fullerene size, and the details can be found in Figure .