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However, achieving selective and direct targeting of mtDNA remains a significant challenge due to its nucleobase similarity to nDNA and necessitates mitochondria-directed delivery strategies. This study reports the identification of a novel N-heterocyclic carbene (NHC) rhenium (Re) complex 4 that selectively targets and damages mtDNA in cancer cells without the need for mitochondria-directed delivery, while sparing nDNA. This remarkable selectivity arises from the inherent reactivity preference of this complex toward mtDNA, rather than from distribution-driven effects. The in vitro potency of complex 4 outperformed that of nDNA-targeting cisplatin. In-depth mechanistic studies revealed that complex 4 forms covalent adducts with mtDNA, leading to disruption of mitochondrial gene replication and transcription. This triggers various downstream effects, including mitochondrial superoxide generation, dissipation of membrane potential, downregulation of nucleoid-associated proteins and polymerase \u03b3 expression, and depletion of OXPHOS proteins and ATP, leading to induction of mitophagy and endoplasmic reticulum stress. It induced necroptosis-mediated cell death and has the ability to overcome cisplatin resistance across multiple cancer cell lines. Furthermore, it significantly reduces the volume of 3D tumor spheroids, demonstrating efficacy in a physiologically relevant tumor model. Overall, this study identifies for the first time the unique mtDNA-targeting capability of [Re(I)(bisNHC)(CO)3Cl] complexes without the need for mitochondria-targeting vectors.<\/jats:p>","DOI":"10.1021\/jacsau.6c00579","type":"journal-article","created":{"date-parts":[[2026,8,18]],"date-time":"2026-08-18T19:02:46Z","timestamp":1787079766000},"page":"4993-5009","source":"Crossref","is-referenced-by-count":0,"title":["Reactivity-Guided\nSelective Covalent Targeting of\nmtDNA over nDNA by an NHC\u2013Rhenium Complex Triggers Bioenergetic\nCollapse in Cancer Cells"],"prefix":"10.1021","volume":"6","author":[{"given":"Amlanjyoti","family":"Dutta","sequence":"first","affiliation":[{"name":"Tata Institute of Fundamental Research , , Homi Bhabha Road , , ,","place":["Mumbai, Maharashtra, India, 400005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shubhangi","family":"Das","sequence":"additional","affiliation":[{"name":"Tata Institute of Fundamental Research , , Homi Bhabha Road , , ,","place":["Mumbai, Maharashtra, India, 400005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sushanta","family":"Chhatar","sequence":"additional","affiliation":[{"name":"Tata Institute of Fundamental Research , , Homi Bhabha Road , , ,","place":["Mumbai, Maharashtra, India, 400005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Parth Sarathi","family":"Nayak","sequence":"additional","affiliation":[{"name":"Tata Institute of Fundamental Research , , Homi Bhabha Road , , ,","place":["Mumbai, Maharashtra, India, 400005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-2928-9882","authenticated-orcid":true,"given":"Subhadeep","family":"Paul","sequence":"additional","affiliation":[{"name":"Tata Institute of Fundamental Research , , Homi Bhabha Road , , ,","place":["Mumbai, Maharashtra, India, 400005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Srinidhi","family":"Srinivasan","sequence":"additional","affiliation":[{"name":"Tata Institute of Fundamental Research , , Homi Bhabha Road , , ,","place":["Mumbai, Maharashtra, India, 400005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3373-6762","authenticated-orcid":true,"given":"Malay","family":"Patra","sequence":"additional","affiliation":[{"name":"Tata Institute of Fundamental Research , , Homi Bhabha Road , , ,","place":["Mumbai, Maharashtra, India, 400005"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,18]]},"reference":[{"issue":"3","key":"2026092808081609500_cit1","doi-asserted-by":"publisher","first-page":"229","DOI":"10.3322\/caac.21834","article-title":"Global Cancer Statistics 2022: GLOBOCAN\nEstimates of Incidence and Mortality Worldwide for 36 Cancers in 185\nCountries","volume":"74","author":"Bray","year":"2024","journal-title":"CA. 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