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Here, Co@CoO heterointerface catalysts are prepared via the controlled reduction of CoO nanosheets. The experimental quantifications of lattice strain and oxygen vacancy concentration on CoO, as well as the charge transfer across the Co\u2013CoO interface are all linearly correlated to the catalytic activity toward the aqueous phase reforming of formaldehyde to produce hydrogen. Mechanistic investigations by spectroscopic measurements and density functional theory calculations elucidate the bifunctional nature of the oxygen\u2010vacancy\u2010rich Co\u2013CoO interfaces, where the Co and the CoO sites are responsible for C\uf8ffH bond cleavage and O\uf8ffH activation, respectively. Optimal catalytic activity is achieved by the sample reduced at 350\u00a0\u00b0C, Co@CoO\u2010350 which exhibits the maximum concentration of Co\u2013CoO interfaces, the maximum concentration of oxygen vacancies, a lattice strain of 5.2% in CoO, and the highest aqueous phase formaldehyde reforming turnover frequency of 50.4 h<jats:sup>\u22121<\/jats:sup> at room temperature. This work provides not only new insights into the strain\u2013vacancy\u2013activity relationship at bifunctional catalytic interfaces, but also a facile synthetic approach to prepare heterostructures with highly tunable catalytic activities.<\/jats:p>","DOI":"10.1002\/smll.202102970","type":"journal-article","created":{"date-parts":[[2021,10,15]],"date-time":"2021-10-15T14:27:17Z","timestamp":1634308037000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":97,"title":["Elucidating the Strain\u2013Vacancy\u2013Activity Relationship on Structurally Deformed Co@CoO Nanosheets for Aqueous Phase Reforming of Formaldehyde"],"prefix":"10.1002","volume":"17","author":[{"given":"Kaicheng","family":"Qian","sequence":"first","affiliation":[{"name":"National Engineering Lab for Textile Fiber Materials and Processing Technology Zhejiang Sci\u2010Tech University  Hangzhou 310018 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