Total volatile basic nitrogen (TVBN), biogenic amine, total viable count (TVC), volatile compounds, and sensory evaluation were conducted to assess the quality of Chinese Mitten Crabs (Eriocheir sinensis) at living, zero, 2, 5, 10, 15, and 24 hr postmortem. The sensory evaluation found a noticeable odor of spoilage becoming evident 10 hr postmortem. The TVBN value increased and then decreased as time increased, reaching 23.67 mg N/100 g at 24 hr postmortem. Although biogenic amines were detected at 5 hr postmortem, by 24 hr postmortem these had not reached dangerous levels of toxicity. The initial TVC (6.06 Log CFU/g) of the living crab samples was relatively high and climbed further postmortem, reaching 10.00 Log CFU/g 24 hr postmortem. Trimethylamine was detected in the living sample in belly meat and 2 hr postmortem in crab roe and reached 8.33 µg/g in the roe 24 hr postmortem. Indole was detected at 0 hr (belly meat) and 10 hr (crab roe) postmortem, but did not change significantly during the observation period. Sulfur‐containing compounds were detected 5 hr after death and gradually increased over the observation period. Most indicators showed major changes at 5 hr and 10 hr postmortem. By 10 hr postmortem, the crab had entered the putrefaction stage and was thus no longer safe for consumption.