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Manufacturing thin sheets and foils of inorganic semiconductors is therefore a bottleneck problem, severely restricting their use in flexible electronic applications. It is recently reported that a few single\u2010crystalline 2D van der Waals (vdW) semiconductors, such as InSe, are deformable under compressive stress. Here it is demonstrated that intralayer fracture toughness can be tailored via compositional design to make inorganic semiconductors processable by cold rolling. Systematic ab initio calculations covering a range of van der Waals semiconductors homologous to InSe are reported, leading to material\u2010property maps that forecast trends in both the susceptibility to interlayer slip and the intralayer fracture toughness against cracking. GaSe is predicted, and experimentally confirmed, to be practically amenable to being rolled to large (three quarters) thickness reduction and length extension by a factor of three. The fracture toughness and cleavage energy are predicted to be 0.25\u00a0MPa\u00a0m<jats:sup>0.5<\/jats:sup> and 15\u00a0meV\u00a0\u00c5<jats:sup>\u22122<\/jats:sup>, respectively. The findings open a new realm of possibility for alloy selection and design toward processing\u2010friendly group\u2010III chalcogenides for practical applications.<\/jats:p>","DOI":"10.1002\/advs.202203776","type":"journal-article","created":{"date-parts":[[2022,8,18]],"date-time":"2022-08-18T21:35:21Z","timestamp":1660858521000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Designing Inorganic Semiconductors with Cold\u2010Rolling Processability"],"prefix":"10.1002","volume":"9","author":[{"given":"Xu\u2010Dong","family":"Wang","sequence":"first","affiliation":[{"name":"Center for Alloy Innovation and Design (CAID) State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University  Xi'an 710049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jieling","family":"Tan","sequence":"additional","affiliation":[{"name":"Center for Alloy Innovation and Design (CAID) State Key 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