Ac lassic challenge in chemical sensingi ss electivity.M etal-organic frameworks (MOFs) are an exciting class of materials because they can be tuned for selective chemical adsorption. Adsorptione ventst riggerw ork-function shifts, which can be detectedw ith ac hemical-sensitive field-effect transistor (power % microwatts). In this work, several case studiesw ere used towards generalizing the sensing mechanism, ultimately towards our metal-centric hypothesis. HKUST-1 was used as ap roof-of-principle humidity sensor.The response is thickness independent, meaning the response is surfacel ocalized. ZIF-8 is demonstrated to be an NO 2 -sensing material,a nd the response is dominated by adsorptiona tm etal sites. Finally, MFM-300(In) shows how standard hard-soft acid-base theory can be used to qualitatively predict sensorr esponses. This paper sets the groundwork for using the tunability of metal-organic frameworks for chemicalsensing with distributed, scalable devices.[a] D.Supporting information and the ORCID identification number(s) for the author(s) of this articlecan be found under: https://doi.