Exposure to morally injurious events may have a severe, prolonged negative impact on psychosocial functioning, known as moral injury (MI). Research into the prevalence of MI has mostly focused on event exposure rather than on psychosocial impact. Also, the relationship between MI and post-traumatic stress disorder (PTSD) remains a matter of interest. The aim of this study was to identify MI and PTSD symptom profiles among trauma-exposed, treatment-seeking police officers and military veterans, and to explore demographic and clinical differences between symptom profiles. Latent class and multinomial regression analyses were conducted in a sample of 1,703 participants, using the Clinician-Administered PTSD Scale for DSM-5 and the Brief Symptom Inventory. Four classes of participants were identified, labeled as a MI class (n = 192; 11.27%), a MI-PTSD class (n = 565; 33.18%), a PTSD class (n = 644; 37.82%), and a Neither MI-nor PTSD class (n = 302; 17.73%), resulting in 44.45% (n = 757) of participants who met an MI symptom profile with or without PTSD. There were significant differences between the classes in terms of gender as well as PTSD and comorbid psychopathology symptom severity, the latter of which was highest in the MI-PTSD class. In conclusion, a substantial subgroup of trauma-exposed, treatment-seeking police officers and military veterans could be classified as suffering from MI. Routinely screening for MI in treatment-seeking police officers and military veterans is recommended, and interventions aimed at relieving MI in these populations may be indicated.