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Cs2O is trigonal omega-like structured and crystallizes in the trigonal R-3m space group. The structure is two-dimensional and consists of three Cs2O sheets oriented in the (0, 0, 1) direction. Cs1+ is bonded in a distorted T-shaped geometry to three equivalent O2- atoms. All Cs–O bond lengths are 2.89 Å. O2- is bonded to six equivalent Cs1+ atoms to form edge-sharing OCs6 octahedra.
Cs2O is zeta iron carbide structured and crystallizes in the orthorhombic Pnnm space group. The structure is three-dimensional. Cs1+ is bonded in a distorted trigonal planar geometry to three equivalent O2- atoms. There are two shorter (2.84 Å) and one longer (3.27 Å) Cs–O bond lengths. O2- is bonded to six equivalent Cs1+ atoms to form a mixture of edge and corner-sharing OCs6 octahedra. The corner-sharing octahedral tilt angles are 52°.