The solvent-free cesium aryloxide complex Cs(O-2,6-i-Pr2C6H3) (1) has been isolated and structurally characterized. In the solid state, 1 consists of Cs(O-2,6-i-Pr2C6H3) units held in pseudo-one-dimensional infinite chains by both Cs-O and Cs-pi-arene interactions with the neighboring unit. The chains are crosslinked into two-dimensional sheets by Cs-C interactions between a carbon atom in the para position of the arene ring and a cesium cation from an adjacent chain.