The purpose of this study was to use multiple assessments to investigate the general versus task-specific characteristics of metacognition in dissimilar chemistry topics. This mixed-method approach investigated the nature of undergraduate general chemistry students' metacognition using four assessments: a self-report questionnaire, assessment of concurrent metacognitive skills, confidence judgment, and calibration accuracy. Data were analyzed using a multitrait-multimethod correlation matrix, supplemented with regression analyses, and qualitative interpretation. Significant correlations among task performance, calibration accuracy, and concurrent metacognition within a task suggest a converging relationship. Confidence judgment, however, was not associated with task performance or the other metacognitive measurements. The results partially support hypotheses of both general and task-specific metacognition. However, general and task-specific properties of metacognition were detected using different assessments. Case studies were constructed for two participants to illustrate how concurrent metacognition varied within different task demands. Considerations of how each assessment may appropriate different metacognitive constructs and the importance of the alignment of analytical constructs when using multiple assessments are discussed. These results may help lead to improvements in metacognition assessment and may provide insights into designs of effective metacognitive instruction.