Unsymmetrical bisfullerene C-131 and its derivatives such as C129BN and C130Si are systematically investigated by semiempirical and density functional theory approaches. In comparison with the experimental data, calculated IR and NMR results reveal that both C-131(H) and C-131(P) isomers are possible compounds to coexist in the synthesized product. The C/Si and CC/BN substitution can change the electronic properties and reactivities compared with the pristine C-131(H) and C-131(P), respectively.