The structure, electronic spectrum, and interatomic interaction parameters of MnB2n (n = 10, 30, 90, 120, 160; M = Mg, Al, Sc, Ti) fullerene-like molecules based on MB2 layered diborides are assessed using quantum-chemical modeling and are analyzed in relation to the atomic configuration, size, and chemical composition of MnB2n. The electronic structure of concentric nanoparticles consisting of M nB2n cage molecules having identical (M10B 20@M90B180) or different (M10B 20@M′90 B180, where M, M′ = Mg, Al) compositions is considered. The results are compared with the electronic properties of crystalline MB2 phases.