The metacognitive self-regulation (MSR) scale is among the most widely used measures of metacognition in educational research. However, the psychometric properties and validity of the scale have not been well established. A series of analyses on a college sample were performed to address this issue. In Study 1, a split-sample exploratory (EFA) and confirmatory factor analysis (CFA) was performed to test the one-factor specification of the MSR scale. Time and study environment (TSE), total study time, and cumulative grade performance average (cGPA) were introduced as outcome variables in a structural equation model (SEM) to examine the factors suggested by the EFA. The results of Study 1 indicated poor one-factor model fit and suggested two and three-factor models provided improved fits of the sample data. Results from the SEM indicated the novel factors from the two and three-factor models had different relationships with the outcome variables than the originally specified one-factor model. In Study 2, a modified one-factor model was introduced that consisted of nine items and was named metacognitive self-regulation revised (MSR-R). Five additional samples were included to replicate the model fit for the revised model specification. Finally, a path analysis was performed to examine the relationship of the MSR-R to variables from Study 1. The results of Study 2 revealed improved psychometric properties and reliability for the MSR-R. An indirect relationship emerged between MSR-R and cGPA through TSE. In conclusion, convincing evidence for replacing the MSR was found and implications of the revised scale for future studies was discussed.