Metacognitive self-knowledge has been identified as a crucial component of effective learning. It entails students recognizing their learning strengths and weaknesses, styles and preferences, and motivational beliefs. The present study explored a method for the development of metacognitive self-knowledge and in doing so, was also a means for discovering what academic experiences students perceive as influential in their development as learners. Twenty-seven college students, all senior psychology majors, produced written narratives in response to a guided reflection activity. A qualitative research approach employing analytic induction was used. Themes of academic experiences as described by participants provided support for neuroscientific findings on learning and active learning pedagogy. In addition, guided reflection was found to be effective for developing metacognitive self-knowledge. However, familiarity with the process of reflection was a crucial factor. This study suggests that educators provide increased opportunities for students to build competency in this regard, referred to as metacognitive literacy.