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Copper (Cu)\u2010based electrocatalysts have shown promise for CO<jats:sub>2<\/jats:sub> conversion into valuable chemicals but are hindered by limited C<jats:sub>2+<\/jats:sub> product selectivity due to competing hydrogen evolution and ineffective dimerization of adsorbed CO intermediate (<jats:sup>*<\/jats:sup>CO). Here, a functional\u2010group\u2010directed strategy is reported to enhance selectivity using single\u2010walled carbon nanotubes (SWCNTs) as supports. The catalytic performance of Cu nanoparticles is strongly influenced by the type and density of functional groups on the SWCNTs. Optimized Cu\/amine\u2010functionalized SWCNTs achieved a Faradaic efficiency of 66.2% and a partial current density of \u2212270\u00a0mA cm<jats:sup>\u22122<\/jats:sup> for C<jats:sub>2<\/jats:sub> products within a flow cell, outperforming Cu\/SWCNTs and Cu\/cyano\u2010functionalized SWCNTs. Density functional theory calculations revealed that the electron\u2010donating amine groups can facilitate electron transfer from the graphite sheet to Cu atoms, thereby shifting the d\u2010band center of Cu upward. This shift enhances <jats:sup>*<\/jats:sup>CO and its hydrogenation derivative adsorption and promotes water splitting, leading to an increased tendency for the generation of C<jats:sub>2<\/jats:sub> products. In situ infrared and Raman spectroscopy confirm the enhancement of key <jats:sup>*<\/jats:sup>CHO intermediate coverage, facilitating C\u2500C coupling. This work provides a molecular framework for exploring interactions between functional groups and active metals in CO<jats:sub>2<\/jats:sub> electrolysis, offering insights for designing catalysts for a broad range of electrocatalytic processes.<\/jats:p>","DOI":"10.1002\/smll.202502733","type":"journal-article","created":{"date-parts":[[2025,4,5]],"date-time":"2025-04-05T09:50:35Z","timestamp":1743846635000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":40,"title":["Functional Group Engineering of Single\u2010Walled Carbon Nanotubes for Anchoring Copper Nanoparticles Toward Selective CO<sub>2<\/sub> Electroreduction to C<sub>2<\/sub> Products"],"prefix":"10.1002","volume":"21","author":[{"given":"Kang","family":"Wang","sequence":"first","affiliation":[{"name":"Institute of Nanochemistry and Nanobiology School of Environmental and Chemical Engineering Shanghai University  99 Shangda Road, BaoShan District Shanghai 200444 P. 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