The present study monitored bacterial succession, physicochemical properties, and volatile organic compounds (VOCs) changes in smoked chicken legs with modified atmosphere packaging (MAP, 60% CO2 and 40% N2) during a 25-day storage period at 4 °C. After 15 days of storage, Serratia proteamaculans and Pseudomonas fragi became the predominant bacteria. Furthermore, physicochemical properties changed significantly, as evidenced by an increase in thiobarbituric acid reactive substances and b* (yellowness) value, and a decrease in hardness. A total of 65 VOCs were identified during storage. Correlation between bacterial succession and quality indicators (including VOCs and physicochemical properties) allowed the identification of 26 core dominant bacteria, including S. proteamaculans, Psychrobacter alimentarius, Pseudomonas putida, and Pseudomonas poae, which were positively related to spoilage VOCs (e.g., 1-octen-3-ol, 1-pentanol, and 3-methyl-1-butanol) and could be defined as specific spoilage organisms (SSOs). The results of this study provide a systematic approach to predict SSOs in smoked chicken legs during storage, which can also provide a basis for product safety.