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Metal-organic framework (MOF) derivatives with unique physicochemical and electronic properties have seen a tremendous growth in diverse applications. Organic optobioelectronics have long been pursued in modern electronics for next-generation bio-relevant implementations. The intersection of these two disciplines could be an appealing way to pursue better performance of materials and devices. Herein this work reports the exploration of MOF derivatives and its ionic modulation for gating organic photoelectrochemical transistor (OPECT) biosensing. In the representative system of poly(ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) gated by zeolitic-imidazolate-framework (ZIF)-8-derived Cd x Zn 1-x S, a high current gain could be achieved at zero gate bias. In connection to a CuO nanoparticle-labeled sandwich immunoassay, acidolysis-triggered Cu2+-induced ionic modulation of the system results into a good performance toward human IgG with a low limit of detection of 0.003 pg/mL. This work features the MOF derivative-gated organic electronics and is expected to inspire more interest to explore various MOF derivative electronics with unknown possibilities, considering the diversity of MOF derivatives. [Display omitted] [ABSTRACT FROM AUTHOR]