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OsB2 crystallizes in the orthorhombic Pmmn space group. The structure is three-dimensional. Os6+ is bonded in a 8-coordinate geometry to eight equivalent B3- atoms. There are a spread of Os–B bond distances ranging from 2.18–2.30 Å. B3- is bonded in a 7-coordinate geometry to four equivalent Os6+ and three equivalent B3- atoms. There is one shorter (1.83 Å) and two longer (1.91 Å) B–B bond length.
BOs is Tungsten Carbide structured and crystallizes in the hexagonal P-6m2 space group. The structure is three-dimensional. Os3+ is bonded to six equivalent B3- atoms to form a mixture of distorted corner, edge, and face-sharing OsB6 pentagonal pyramids. All Os–B bond lengths are 2.21 Å. B3- is bonded to six equivalent Os3+ atoms to form a mixture of distorted corner, edge, and face-sharing BOs6 pentagonal pyramids.
Os3B crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Os1- is bonded to eight equivalent Os1- and four equivalent B3+ atoms to form distorted OsB4Os8 cuboctahedra that share corners with four equivalent BOs12 cuboctahedra, corners with fourteen equivalent OsB4Os8 cuboctahedra, edges with six equivalent BOs12 cuboctahedra, edges with twelve equivalent OsB4Os8 cuboctahedra, faces with four equivalent BOs12 cuboctahedra, and faces with sixteen equivalent OsB4Os8 cuboctahedra. There are a spread of Os–Os bond distances ranging from 2.59–2.87 Å. There are two shorter (2.51 Å) and two longer (2.73 Å) Os–B bond lengths. B3+ is bonded to twelve equivalent Os1- atoms to form BOs12 cuboctahedra that share corners with six equivalent BOs12 cuboctahedra, corners with twelve equivalent OsB4Os8 cuboctahedra, edges with eighteen equivalent OsB4Os8 cuboctahedra, faces with eight equivalent BOs12 cuboctahedra, and faces with twelve equivalent OsB4Os8 cuboctahedra.