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Problem gambling and gambling disorder (GD) are associated with a range of mental health concerns that extend beyond gambling behaviors alone. Prior works have consistently linked gambling disorder with symptoms of posttraumatic stress disorder (PTSD), both cross-sectionally and over time. However, very little work has examined the specific relationships between these 2 disorders. The present work postulated that symptoms of PTSD are likely associated with unique beliefs about gambling behaviors and unique motivations to gamble. Using 2 samples—an inpatient sample of U.S. Armed Forces veterans (N = 332) seeking treatment for GD and a Web-sample of gambling adults (N = 589)—we examined these ideas. Results from both samples indicated that symptoms of PTSD were related to positive gambling expectancies and coping motivations for gambling. Additionally, in both samples, positive gambling expectancies were associated with greater coping motivations for gambling. Structural equation models revealed that positive gambling expectancies were consistently associated with coping motivations for gambling. The findings indicate that symptoms of PTSD are likely associated with unique beliefs about and motivations for gambling behaviors. Given the high comorbidity between symptoms of PTSD and GD, these specific relationships are likely of clinical interest in populations seeking treatment for either PTSD or for problems with gambling behaviors.