The structures, relative stabilities, vertical detachment energies and exchange coupling constants of a series of Mn-based dinuclear superhalogens and their isoelectronic analogues are explored via combined DFT and Broken-Symmetry study.Both the capabilities of various XC functionals and basis sets effect are investigated.The large magnitudes of calculated exchange coupling con-stants indicate the apparent molecular magnetism of this new type of superhalogens.Moreover, the high degree of possibility for the coexistence of both higher stability and stronger magnetic coupling in TM-based polynuclear superhalogens is also confirmed.Besides these, the larger magnitudes of the calculated coupling constants of iron-based clusters here, compared with [Mn2C15]-cluster, demonstrate the possibility of the existence of strong magnetic coupling in potential iron-based homo-and heterodinuclear superhalogens.The analysis of spin density distribution is also performed to understand the mechanisms of magnetic exchange coupling.