A novel food processing technique based on the combination of cold atmospheric plasma (CAP) and chitosan oligosaccharide treatment (COS) was developed to enhance antibacterial performance and extend the shelf life of Pacific white shrimp (Litopenaeus vannamei). Effects of different treatments on the microbial community composition, physicochemical properties, and post-storage behaviors of Pacific white shrimp were evaluated during chilled storage for up to 10 days. Results showed that the synergistic effects of COS and CAP could be obtained, largely inhibiting the growth of microorganisms. The content of total volatile basic nitrogen (TVB-N), total viable counts (TVC), and pH value in treated groups were lower than in the control group and the loss of moisture content, water activity, and sensory score were observed. Compared to the control group, shrimp was on the verge of spoilage on the 6th day of storage, while the COS–CAP-treated shrimp had a 4-day lag period. Moreover, the COS and CAP could effectively inhibit the growth ofAliivibrio, the predominant microbial group in the ultimate storage period. This study suggests that the combined utilization of COS and CAP could be a high-efficacy technique for extending the shelf-life of shrimp.