Numerous studies demonstrate the importance of self-regulation during learning by problem-solving. Recent work in learning analytics has largely examined students' use of SRL concerning overall learning gains. Limited research has related SRL to in-the-moment performance differences among learners. The present study investigates SRL behaviors in relationship to learners' moment-by-moment performance while working with intelligent tutoring systems for stoichiometry chemistry. We demonstrate the feasibility of labeling SRL behaviors based on AI-generated think-aloud transcripts, identifying the presence or absence of four SRL categories (processing information, planning, enacting, and realizing errors) in each utterance. Using the SRL codes, we conducted regression analyses to examine how the use of SRL in terms of presence, frequency, cyclical characteristics, and recency relate to student performance on subsequent steps in multi-step problems. A model considering students' SRL cycle characteristics outperformed a model only using in-the-moment SRL assessment. In line with theoretical predictions, students' actions during earlier, process-heavy stages of SRL cycles exhibited lower moment-by-moment correctness during problem-solving than later SRL cycle stages. We discuss system re-design opportunities to add SRL support during stages of processing and paths forward for using machine learning to speed research depending on the assessment of SRL based on transcription of think-aloud data.