We used nationwide population-based data to identify optimal hospital and surgeon volume thresholds and to discover the effects of these volume thresholds on operative mortality and length of stay (LOS) for coronary artery bypass surgery (CABG). Retrospective cohort study. General acute care hospitals throughout Taiwan. A total of 12,892 CABG patients admitted between 2011 and 2015 were extracted from Taiwan National Health Insurance claims data. Operative mortality and LOS. Restricted cubic splines were applied to discover the optimal hospital and surgeon volume thresholds needed to reduce operative mortality. Generalized estimating equation regression modeling, Cox proportional-hazards modeling and instrumental variables analysis were employed to examine the effects of hospital and surgeon volume thresholds on the operative mortality and LOS. The volume thresholds for hospitals and surgeons were 55 cases and 5 cases per year, respectively. Patients who underwent CABG from hospitals that did not reach the volume threshold had higher operative mortality than those who received CABG from hospitals that did reach the volume threshold. Patients who underwent CABG with surgeons who did not reach the volume threshold had higher operative mortality and LOS than those who underwent CABG with surgeons who did reach the volume threshold. This is the first study to identify the optimal hospital and surgeon volume thresholds for reducing operative mortality and LOS. This supports policies regionalizing CABG at high-volume hospitals. Identifying volume thresholds could help patients, providers, and policymakers provide optimal care.