Harnessing the ability of microorganisms to fix, convert and utilize CO2 for chemical production has important implications for global carbon reduction. In this study, carbonic anhydrase (CA) and/or phosphoenolpyruvate carboxykinase (PEPCK) were overexpressed in Corynebacterium acetoacidophilum. A process was established to capture CO2 and convert it into succinic acid (SA) from the off-gas produced by Saccharomyces cerevisiae fermenting ethanol (EtOH), using the engineered strain of C. acetoacidophilum. By constructing a coupling device and optimizing the ratio of working medium volumes in the two-chamber bioreactor, the maximum yields of EtOH and SA from glucose were 0.51 g/g and 0.70 g/g, respectively. A scale-up trial was performed in a 3-L fermenter and calculation of the environmental factors demonstrated that the linked-fermentation strategy was more environmentally-friendly than conventional SA fermentation, indicating potential for industrial application.