Purpose Medication non-adherence is a huge concern for the medical community. For chronic, especially neurological diseases, taking medication is a central pillar of treatment. To improve adherence to these oftentimes complex medication regimens, the construct needs to be understood in more depth. The aim of this study was to investigate associations between adherence with sociodemographics, clinical variables, and coping in neurological patients. Patients and Methods The sample consisted of 545 patients from a German neurological clinic. Adherence was assessed with the Stendal Adherence to Medication Score (SAMS). Patients were grouped as completely adherent (SAMS = 0), non-adherent (upper 25% of the sample), and moderately adherent. Associations with coping were assessed using the Essen Coping Questionnaire. Results Medication adherence was low compared to other non-neurological patient samples. Differences between adherence groups were found regarding gender and facets of coping, namely “trivialisation, wishful thinking and defence” and “finding of inner stability”. Conclusion Interventions to improve medication adherence should focus on facets of coping with disease, increasing acceptance of disease, willpower, and confidence in treatment.