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Valley degree of freedom exists in a few conventional semiconductors, but recently the emerging 2D materials, such as monolayer transition\u2010metal dichalcogenides (TMDs), are considered more ideal for valleytronics, due to the additional protection from spin\u2010valley locking enabled by their inversion symmetry breaking and large spin\u2010orbit coupling. However, current limitations in the valley lifetime, operation temperature, and light\u2010valley conversion efficiency in existing materials encumber the practical applications of valleytronics. In this article, the valley depolarization mechanisms and recent progress of novel materials are systematically reviewed for valleytronics beyond TMDs. Valley physics is first reviewed and the factors determining the valley lifetime, including the intrinsic electron\u2010electron and electron\u2010lattice interactions, as well as extrinsic defect effects. Then, experimentally demonstrated and theoretically proposed valley materials are introduced which potentially improve valley properties through the changes of spin\u2010orbit coupling, electronic interactions, time\u2010reversal symmetry, structures, and defects. Finally, the challenges and perspectives are summarized to realize valleytronic devices in the future.<\/jats:p>","DOI":"10.1002\/smll.202402139","type":"journal-article","created":{"date-parts":[[2024,11,29]],"date-time":"2024-11-29T02:06:19Z","timestamp":1732845979000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Valleytronics: Fundamental Challenges and Materials Beyond Transition Metal Chalcogenides"],"prefix":"10.1002","volume":"21","author":[{"given":"Rui","family":"Xu","sequence":"first","affiliation":[{"name":"Department of Materials Science and NanoEngineering Rice University  Houston Texas 77005 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiguo","family":"Zhang","sequence":"additional","affiliation":[{"name":"Department of Materials Science Fudan University  Shanghai 200433 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