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MnB4 crystallizes in the orthorhombic Immm space group. The structure is three-dimensional. Mn is bonded to twelve equivalent B atoms to form a mixture of edge and face-sharing MnB12 cuboctahedra. There are four shorter (2.06 Å) and eight longer (2.19 Å) Mn–B bond lengths. B is bonded in a 7-coordinate geometry to three equivalent Mn and four equivalent B atoms. There are a spread of B–B bond distances ranging from 1.71–1.88 Å.
MnB4 crystallizes in the monoclinic P2_1/c space group. The structure is three-dimensional. Mn is bonded in a 12-coordinate geometry to twelve B atoms. There are a spread of Mn–B bond distances ranging from 2.00–2.31 Å. There are four inequivalent B sites. In the first B site, B is bonded in a 7-coordinate geometry to three equivalent Mn and four B atoms. There are a spread of B–B bond distances ranging from 1.69–1.85 Å. In the second B site, B is bonded in a 7-coordinate geometry to three equivalent Mn and four B atoms. There are a spread of B–B bond distances ranging from 1.73–1.89 Å. In the third B site, B is bonded in a 8-coordinate geometry to three equivalent Mn and five B atoms. The B–B bond length is 2.08 Å. In the fourth B site, B is bonded in a 8-coordinate geometry to three equivalent Mn and five B atoms.