Applications of porous metal-org. frameworks (MOFs) in electronic devices are rare, owing in large part to a lack of MOFs that display elec. cond. Here, we describe the use of conductive two-dimensional (2D) MOFs as a new class of materials for chemiresistive sensing of volatile org. compds. (VOCs). We demonstrate that a family of structurally analogous 2D MOFs can be used to construct a cross-reactive sensor array that allows for clear discrimination between different categories of VOCs. Exptl. data show that multiple sensing mechanisms are operative with high degrees of orthogonality, establishing that the 2D MOFs used here are mechanistically unique and offer advantages relative to other known chemiresistor materials.