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Here, a multiferroic morphotropic phase boundary (MPB) is demonstrated\u00a0wherein the crystal structure, polarization, and magnetic order simultaneously evolve across a chemically induced phase boundary in strain\u2010engineered (1\u2212\n                    <jats:italic>x<\/jats:italic>\n                    )BiFeO\n                    <jats:sub>3<\/jats:sub>\n                    \u2010(\n                    <jats:italic>x<\/jats:italic>\n                    )BaTiO\n                    <jats:sub>3<\/jats:sub>\n                    thin films. Between 0.1 &lt;\n                    <jats:italic>x<\/jats:italic>\n                    &lt; 0.2, the crystal structure evolves from a monoclinic phase to a newly stabilized tetragonal phase through an intermediate mixed\u2010phase region. This structural transition is accompanied by concurrent changes in magnetic order, resulting in dramatically enhanced functional responses as compared with those of BiFeO\n                    <jats:sub>3<\/jats:sub>\n                    . Specifically, films with\n                    <jats:italic>x<\/jats:italic>\n                    = 0.2 exhibit larger electromechanical strains (\u2248 0.3%, about three\u2010times larger than BiFeO\n                    <jats:sub>3<\/jats:sub>\n                    ) and a significantly enhanced magnetoelectric\u2010coupling coefficient (\u03b1\n                    <jats:sub>ME<\/jats:sub>\n                    \u2248 416\u00a0mV cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    Oe\n                    <jats:sup>\u22121<\/jats:sup>\n                    , nearly 1000\u2010 and 19\u2010times larger than bulk and thin\u2010film BiFeO\n                    <jats:sub>3<\/jats:sub>\n                    , respectively). These enhancements diminish beyond the MPB (\n                    <jats:italic>x<\/jats:italic>\n                    &gt; 0.2) and arise from polarization rotation and evolving spin configurations driven by the near degeneracy of competing ferroic states at the multiferroic MPB. These results establish a rare multiferroic MPB where both the polar and magnetic order evolve simultaneously, providing a promising strategy for designing materials with strongly coupled ferroic order parameters.\n                  <\/jats:p>","DOI":"10.1002\/adma.74920","type":"journal-article","created":{"date-parts":[[2026,9,5]],"date-time":"2026-09-05T17:03:05Z","timestamp":1788627785000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["A Multiferroic Morphotropic Phase Boundary"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-5628-505X","authenticated-orcid":false,"given":"Tae Yeon","family":"Kim","sequence":"first","affiliation":[{"name":"Department of Materials Science and NanoEngineering Rice University  Houston TX USA"},{"name":"Rice Advanced Materials Institute Rice University  Houston TX 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Materials Science and Engineering University of California  Berkeley CA USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9448-4370","authenticated-orcid":false,"given":"Liyan","family":"Wu","sequence":"additional","affiliation":[{"name":"Department of Mechanical Engineering and Mechanics Drexel University  Philadelphia PA USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0524-1332","authenticated-orcid":false,"given":"Ramamoorthy","family":"Ramesh","sequence":"additional","affiliation":[{"name":"Department of Materials Science and NanoEngineering Rice University  Houston TX USA"},{"name":"Rice Advanced Materials Institute Rice University  Houston TX USA"},{"name":"Department of Materials Science and Engineering University of California  Berkeley CA 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