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While the performance of such heterojunctions is strongly governed by their built-in electric field and interfacial band alignment, strategies for actively tuning these parameters in printed bulk heterojunctions have remained largely unexplored. In this regard, here we show an inkjet-printed bulk heterojunction diode with semiconducting amorphous indium gallium oxide (a-IGO) and conducting poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS), whose interfacial barrier can be dynamically modulated by a solvent (dimethyl sulfoxide, DMSO) or a composite solid polymer electrolyte (CSPE). Systematic studies of pristine, DMSO-treated, and CSPE-treated devices reveal that DMSO enhances charge transport in PEDOT:PSS, while mobile ions of CSPE penetrate the polymer matrix and accumulate at the heterojunction interface. Capacitance\u2013voltage measurements show that ionic screening increases the built-in potential from 0.36 to 0.70 eV by inducing additional band bending within a-IGO. Consequently, the off-current decreases by more than two orders of magnitude, accompanied by a substantial enhancement in rectification ratio. The strengthened junction field promotes efficient separation of photogenerated carriers under ultraviolet illumination, increasing the photosensitivity from 103 to beyond 106 while achieving a responsivity of 80 A\/W, a specific detectivity of 0.25 \u00d7 1012 Jones, and an external quantum efficiency of 27200%. This elevated built-in potential further enables zero-biased ultraviolet photodetection with a photosensitivity of \u223c104 and a responsivity of 45 mA\/W. Furthermore, a three-terminal electrolyte-gated device can demonstrate ion-induced modulation of the interfacial barrier, enabling a transition from rectifying to near-Ohmic behavior and thereby realizing a tuneable diode. This electrolyte-assisted ionic-modulation strategy enables reconfigurable hybrid heterojunctions for next-generation, energy-efficient sensing and multifunctional optoelectronic applications.<\/jats:p>","DOI":"10.1021\/acsami.6c12401","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T11:01:35Z","timestamp":1791370895000},"page":"56287-56298","source":"Crossref","is-referenced-by-count":0,"title":["Electrolyte-Induced Band Bending and Barrier Tuning to Enhance Photodetection in Inkjet-Printed Organic\u2013Inorganic Heterojunctions"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-9985-8148","authenticated-orcid":true,"given":"Manvendra","family":"Singh","sequence":"first","affiliation":[{"name":"Indian Institute of Science (IISc) , , C V Raman Avenue , , ,","place":["Bangalore, Karnataka, India, 560012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mohammed Hadhi Pazhaya","family":"Puthanveettil","sequence":"additional","affiliation":[{"name":"Indian Institute of Science (IISc) , , C V Raman Avenue , , ,","place":["Bangalore, Karnataka, India, 560012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3952-2952","authenticated-orcid":true,"given":"Subho","family":"Dasgupta","sequence":"additional","affiliation":[{"name":"Indian Institute of Science (IISc) , , C V Raman Avenue , , ,","place":["Bangalore, Karnataka, India, 560012"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,7]]},"reference":[{"issue":"5","key":"2026102609072879400_cit1","doi-asserted-by":"publisher","first-page":"4895","DOI":"10.1021\/acsnano.6b01842","article-title":"Contacts between Two- and Three-Dimensional Materials: Ohmic, Schottky, and p \u2013 n Heterojunctions","volume":"10","author":"Xu","year":"2016","journal-title":"ACS Nano"},{"issue":"3","key":"2026102609072879400_cit2","doi-asserted-by":"publisher","first-page":"435","DOI":"10.1002\/j.1538-7305.1949.tb03645.x","article-title":"The Theory of p-n Junctions in Semiconductors and p-n Junction Transistors","volume":"28","author":"Shockley","year":"1949","journal-title":"Bell Syst. 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