In the context of the “Dual carbon” strategy, green and low-carbon development has become a necessary route for the aerospace manufacturing industry development. Surface treatment process, as a key process of large aircraft parts processing, is characterized by multiple processing procedure, long processing flow, and multiple carbon emission sources, and there are problems of high energy consumption, low energy efficiency, and severe carbon emissions, which poses challenges to its green and low-carbon development. To this end, this study takes the surface treatment process of large aircraft parts as an object to define the carbon emission boundary of the surface treatment process, and analyze the carbon emission characteristics of this process. On this basis, a carbon emission accounting method for the surface treatment process of large aircraft parts based on the improved value stream mapping is proposed, and the carbon emission hotspot is obtained to elucidate the carbon reduction potential of the surface treatment process based on the sensitivity analysis. Finally, the boric-sulfuric acid anodic oxidation of the large aircraft aluminum alloy parts is performed to verify the effectiveness of the proposed method. This research can provide methodological support for the refined carbon emission modeling for surface treatment process, and also lays a theoretical foundation for the subsequent development of energysaving and carbon-reducing strategies.