Religious and spiritual struggles are typically assessed by self-report scales using closed-ended items, yet nascent research suggests that using open-ended interviews and prompts may complement and advance assessment and theories. In the current mixed-methods study, undergraduate participants (N = 976) completed open-ended descriptions of their religious and spiritual struggles, the Religious and Spiritual Struggles Scale (RSS), and a quantitative measure of religious belief salience. Qualitative description showed that the themes emerging from open-ended descriptions generally fell within the broad domains of the RSS though some descriptions reflected more contextualized struggles. Scores derived from the open-ended responses to assess RSS domains achieved evidence of reliability, and quantitative correlational analyses provided support for convergent and discriminant validity with the RSS. Correlations revealed a mix of similar and divergent associations between methods of assessing religious and spiritual struggles and religious belief salience. Open-ended descriptions of religious and spiritual struggles may yield reliable and valid information that is related to but distinct from assessments relying on closed-ended items.