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Up to now, activated substrates (such as styrene and butadiene derivatives) have been predominantly focused on due to their high activity. In contrast, the unactivated substrates, with low reductive potentials and unstable radical intermediates but more abundant in nature and industry, have rarely been employed. Herein, we proposed a nickel\u2010electrocatalytic system for the regioconvergent carboxylation of unactivated olefins or halides. Various carboxylic acids were obtained by the remote hydro\u2010 or di\u2010carboxylation under mild reaction conditions with inexpensive catalysts and electrodes. It was noteworthy that readily available alkanes could also be utilized as starting substrates for the site\u2010selective electrocarboxylation process by the unified catalytic strategy. This method expands the scope of organic molecules coupled with CO\n                    <jats:sub>2<\/jats:sub>\n                    , and demonstrates the possibility of ectopic and remote C\u2500H carboxylation. Mechanistic investigations indicated that the Ni\u2500H species generated in the Ni\u2010electrocatalytic system play a key role for promoting chain walking to efficiently produce activated olefin intermediates, which subsequently undergo radical addition with CO\n                    <jats:sub>2<\/jats:sub>\n                    radical anion and further transform into the desired products.\n                  <\/jats:p>","DOI":"10.1002\/anie.202518160","type":"journal-article","created":{"date-parts":[[2025,12,2]],"date-time":"2025-12-02T07:00:50Z","timestamp":1764658850000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Electrocatalytic Migratory Carboxylation of Unactivated Olefins or Halides with CO\n                    <sub>2<\/sub>"],"prefix":"10.1002","volume":"65","author":[{"given":"Mengke","family":"Dong","sequence":"first","affiliation":[{"name":"Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular &amp; Process Engineering, School of Chemistry and Molecular Engineering East China Normal University  Shanghai 200062 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongwu","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Petroleum Molecular and Process Engineering, SKLPMPE Sinopec Research Institute of Petroleum Processing Co., LTD.  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