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Despite recent advancements, precise control over multiple signaling molecules within a single platform remains challenging. Here, we introduce a bioelectrosynthesis approach capable of selectively producing two types of signaling molecules from a single precursor. This system leverages multi\u2010metal sulfide electrocatalysts inspired by denitrifying enzymes, which generate signaling molecules, nitric oxide (NO), and ammonia (NH\n                    <jats:sub>3<\/jats:sub>\n                    ) from nitrite ions. By controlling catalytic active sites, NO or NH\n                    <jats:sub>3<\/jats:sub>\n                    can be selectively produced under mild electric fields in physiologically relevant conditions. In situ product analyses and first\u2010principles calculations reveal that NO intermediate binding affinity determines product selectivity. These electrocatalysts integrate seamlessly with biological systems, allowing precise, on\u2010demand modulation of NO\u2010 or NH\n                    <jats:sub>3<\/jats:sub>\n                    \u2010mediated signaling pathways in human cell lines. By combining electrochemical precision with selective cell control, this strategy may advance the study and regulation of biological systems.\n                  <\/jats:p>","DOI":"10.1002\/anie.202508192","type":"journal-article","created":{"date-parts":[[2025,7,8]],"date-time":"2025-07-08T14:07:54Z","timestamp":1751983674000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Bioelectrosynthesis of Signaling Molecules for Selective Modulation of Cell Signaling"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-2806-6895","authenticated-orcid":false,"given":"Myeongeun","family":"Lee","sequence":"first","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and Technology (KAIST)  Daejeon 34141 South 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