Metal-organic frameworks (MOFs) are a promising class of porous materials for the design of gas sensing arrays, which are often called electronic noses. Due to their chemical and structural tunability, MOFs are a highly diverse class of materials that align well with the similarly diverse class of volatile organic compounds (VOCs) of interest in many gas detection applications. In principle, by choosing the right combination of cross-sensitive MOFs, layered on appropriate signal transducers, one can design an array that yields detailed information about the composition of a complex gas mixture. However, despite the vast number of MOFs from which one can choose, gas sensing arrays that rely too heavily on distinct chemistries can be impractical from the cost and complexity perspective. On the other hand, it is difficult for small arrays to have the desired selectivity and sensitivity for challenging sensing applications, such as detecting weakly adsorbing gases with weak signals, or conversely, strongly adsorbing gases that readily saturate MOF pores. In this work, we employed gas adsorption simulations to explore the use of a variable pressure sensing array as a means of improving both sensitivity and selectivity as well as increasing the information content provided by each array. We studied nine different MOFs (HKUST-1, IRMOF-1, MgMOF-74, MOF-177, MOF-801, NU-100, NU-125, UiO-66, and ZIF-8) and four different gas mixtures, each containing nitrogen, oxygen, carbon dioxide, and exactly one of the hydrogen, methane, hydrogen sulfide, or benzene. We found that by lowering the pressure, we can limit the saturation of MOFs, and by raising the pressure, we can concentrate weakly adsorbing gases, in both cases, improving gas detection with the resulting arrays. In many cases, changing the system pressure yielded a better improvement in performance (as measured by the Kullback-Liebler divergence of gas composition probability distributions) than including additional MOFs. We thus demonstrated and quantified how sensing at multiple pressures can increase information content and cross-sensitivity in MOF-based arrays while limiting the number of unique materials needed in the device.