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Herein, a series of hierarchical hollow VS&amp;Si-CuInS2\/SiC-X heterojunctions with abundant S and Si vacancies were designed, synthesized, and utilized for photoelectrocatalytic CO2 reduction in an aqueous KHCO3 solution. Our results reveal that the unique hierarchical hollow architecture, S and Si vacancies, and n\u2212n heterojunction property synergistically contribute to CO2 reduction performance and selectivity to C2 products. In particular, the optimal heterojunction VS&amp;Si-CuInS2\/SiC-2 achieves a generation rate of 79.38 \u03bcM h\u22121 cm\u22122 for carbon-based products and a C2 selectivity of 83.63% for liquid products. Moreover, its total electron transfer rate (263.19 \u03bcM h\u22121 cm\u22122) is 3.60 times higher than that of VSi-SiC and 3.96 times higher than that of VS-CuInS2, respectively. DFT calculations indicate that the S and Si vacancies can evidently reduce the reaction barriers in the CO2 reduction, promoting the generation of crucial intermediates and facilitating the C\u2212C coupling reaction on the catalyst surface. Based on the key intermediates *\u2550C\u2550O, *CHO, *COCHO, and *COCH3 detected through in situ FTIR spectroscopy and confirmed by DFT calculations, a dual-vacancy-assisted mechanism is proposed for photoelectrocatalytic CO2 reduction.<\/jats:p>","DOI":"10.1021\/acsami.6c13125","type":"journal-article","created":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T20:46:51Z","timestamp":1788468411000},"page":"49213-49224","source":"Crossref","is-referenced-by-count":0,"title":["Building VS&amp;Si-CuInS2\/SiC Heterojunctions Mimicking Thylakoid for Artificial Photosynthesis\u2014Dual-Vacancy-Assisted Mechanism"],"prefix":"10.1021","volume":"18","author":[{"given":"Chenpu","family":"He","sequence":"first","affiliation":[{"name":"Lanzhou University , , , ,","place":["Lanzhou, Gansu, P. R. 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