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Objective: Posttraumatic embitterment disorder (PTED) comprises a stress-related response to a negative life event that violates the belief system of the individual. Characteristic symptoms involve repeated intrusive thoughts, emotional arousal when reminded of the event, and decreases in well-being. Method: Within the scope of the present study, embitterment was treated as a continuous rather than categorical concept, and we investigated its psychological and brain structural correlates in a sample of healthy older adults. Results: We found a negative association between the PTED self-rating score and self-reported well-being, life satisfaction, and future time perspective and a positive association with loneliness, perceived stress, chronic strain, and external control beliefs. We found no significant association between embitterment and brain regions that have been associated with stress exposure and posttraumatic stress disorder (PTSD)—hippocampus and the medial prefrontal cortex. This may emphasize the fundamental difference between PTED and PTSD. In a whole-brain analysis, we found a positive correlation between embitterment and gray matter volume in the precuneus and white matter volume in the bilateral uncinate fasciculus. Conclusions: The precuneus and uncinate fasciculus are brain regions that have been related to episodic memory retrieval, matching well to the symptoms of intrusive thoughts and an overwhelming preoccupation with the event that caused the PTED. Further longitudinal research is needed to unravel whether these structural correlates represent preconditions or rather the consequence of embitterment.