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In van der Waals heterostructures, such transfer can be enabled by type\u2010III band alignment together with magnetic\u2010field\u2010induced spin polarization of the bands in adjacent magnetic layers. Yet, continuous and robust valley control with high magnetic\u2010field susceptibility remains challenging, particularly beyond binary switching in out\u2010of\u2010plane easy\u2010axis magnets. Here we fabricate a CrSBr\/WSe\n                    <jats:sub>2<\/jats:sub>\n                    \/CrSBr heterostructure, where two semiconductor\u2010magnet interfaces promote efficient hot\u2010carrier transfer. Utilizing valley\u2010resolved magneto\u2010photoluminescence spectroscopy, we reveal a pronounced field\u2010sign\u2010asymmetric response and a magnetic\u2010state\u2010dependent evolution of emergent spectral features that track the spin configuration of multilayer CrSBr via spin\u2010selective hot\u2010carrier transfer. This mechanism enables giant, continuous tuning, and magnetic\u2010state\u2010dependent reversal of the degree of circular polarization (DoCP), reaching \u223c 40% for excitons and \u223c 80% for trion emission. Our results establish spin\u2010polarized interlayer hot\u2010carrier transfer as an efficient knob for engineering valley polarization and coherence in TMDs, and highlight antiferromagnet\u2010based stacks as a versatile platform for magnetically programmable quantum optoelectronic functionalities.\n                  <\/jats:p>","DOI":"10.1002\/adma.75103","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T03:19:40Z","timestamp":1790738380000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Giant Nonequilibrium Valley Control via Spin\u2010Selective Hot\u2010Carrier Transfer in an Antiferromagnetic van der Waals Stack"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-2886-5929","authenticated-orcid":false,"given":"Ke","family":"Xiao","sequence":"first","affiliation":[{"name":"NISE Department Max Planck Institute of Microstructure Physics  Halle (Saale) Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiabao","family":"Yang","sequence":"additional","affiliation":[{"name":"NISE Department Max Planck Institute of Microstructure Physics  Halle (Saale) Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kai","family":"Feng","sequence":"additional","affiliation":[{"name":"Physics Department and State Ley Laboratory of Quantum Optical Materials The University of Hong Kong  Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yicheng","family":"Guan","sequence":"additional","affiliation":[{"name":"NISE Department Max Planck Institute of Microstructure Physics  Halle (Saale) Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"James Caleb","family":"Peters","sequence":"additional","affiliation":[{"name":"NISE Department Max Planck Institute of Microstructure Physics  Halle (Saale) Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ramona","family":"Hoffmann","sequence":"additional","affiliation":[{"name":"NISE Department Max Planck Institute of Microstructure Physics  Halle (Saale) Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Niels","family":"Schr\u00f6ter","sequence":"additional","affiliation":[{"name":"NISE Department Max Planck Institute of Microstructure Physics  Halle (Saale) Germany"},{"name":"Martin\u2010Luther\u2010Universit\u00e4t Halle\u2010Wittenberg  Halle (Saale) Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4702-6139","authenticated-orcid":false,"given":"Stuart S. 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