A novel atomically synergistic binuclear-site catalyst (ABC) composed of Zn^δ+–O–Cr^6+ on zeolite SSZ-13 is developed for the iso-stoichiometric co-conversion of ethane and CO₂ to ethylene and CO. This catalyst exhibits exceptional performance, achieving 100% ethylene selectivity and 99.0% CO₂ utilization under 500 °C with 9.6% ethane conversion. The synergistic effects between acidic Zn and redox Cr sites are crucial for the catalytic process. Zn^δ+ sites facilitate β-C-H bond cleavage in ethane and the formation of Zn-H^δ hydride, enhancing CO₂ adsorption and preventing ethane C-C bond scission. Redox Cr sites accelerate CO₂ dissociation and promote H₂O formation/desorption. In-situ/ex-situ spectroscopic studies and DFT calculations reveal the atomic synergies between Zn and Cr sites. The ABC catalyst demonstrates higher catalytic activity compared to pure Zn and Cr catalysts, with a 1.5- and 4-fold increase in ethane dehydrogenation and CO₂ conversion, respectively. The catalyst's performance is attributed to the unique atomic synergies within the Zn^δ+–O–Cr^6+ site, which enables efficient ethane and CO₂ conversion. The ABC catalyst also shows excellent stability and regeneration ability, maintaining high ethylene selectivity and CO₂ utilization over 150 hours. The study highlights the importance of atomic synergy in catalyst design, offering a pathway for the development of advanced catalysts for CO₂ conversion and olefin production.A novel atomically synergistic binuclear-site catalyst (ABC) composed of Zn^δ+–O–Cr^6+ on zeolite SSZ-13 is developed for the iso-stoichiometric co-conversion of ethane and CO₂ to ethylene and CO. This catalyst exhibits exceptional performance, achieving 100% ethylene selectivity and 99.0% CO₂ utilization under 500 °C with 9.6% ethane conversion. The synergistic effects between acidic Zn and redox Cr sites are crucial for the catalytic process. Zn^δ+ sites facilitate β-C-H bond cleavage in ethane and the formation of Zn-H^δ hydride, enhancing CO₂ adsorption and preventing ethane C-C bond scission. Redox Cr sites accelerate CO₂ dissociation and promote H₂O formation/desorption. In-situ/ex-situ spectroscopic studies and DFT calculations reveal the atomic synergies between Zn and Cr sites. The ABC catalyst demonstrates higher catalytic activity compared to pure Zn and Cr catalysts, with a 1.5- and 4-fold increase in ethane dehydrogenation and CO₂ conversion, respectively. The catalyst's performance is attributed to the unique atomic synergies within the Zn^δ+–O–Cr^6+ site, which enables efficient ethane and CO₂ conversion. The ABC catalyst also shows excellent stability and regeneration ability, maintaining high ethylene selectivity and CO₂ utilization over 150 hours. The study highlights the importance of atomic synergy in catalyst design, offering a pathway for the development of advanced catalysts for CO₂ conversion and olefin production.