I sin højest profilerede kamp i sin karriere mødte Smith [[Jon Jones]] om UFC Light Heavyweight Championship den 2. marts 2019, på UFC 235.<ref>{{Kilde nyheder|url=http://www.sherdog.com/news/news/Jon-Jones-to-Defend-Light-Heavyweight-Crown-vs-Anthony-Smith-in-UFC-235-Headliner-147855|title=Jon Jones to defend light heavyweight crown vs. Anthony Smith in UFC 235 headliner|last=Tristen Critchfield|date=2019-01-06|access-date=2019-01-07|publisher=sherdog.com}}</ref> Han tabte kampen via [[enstemmig afgørelse]]. <ref>{{Cite journal|title=ASSESSMENT OF DESIGN REQUIREMENTS  AGAINST PROGRESSIVE COLLAPSE IN  UFC 4-023-03: NUMERICAL SIMULATION|url=http://dx.doi.org/10.18057/ijasc.2018.14.4.1}}</ref>
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