Using the Internet as a learning tool has great promise, but also poses significant challenges. Theories and research confirm the importance of students' engagement in self-regulated learning processes for effective Internet learning. In this article the Authors describe a structured think-aloud procedure intended to support students' engagement in proactive self-regulated learning processes when learning on the Internet. The structured think-aloud requires students to self-regulate their learning by verbalizing their plans and evaluating their actions to achieve their online learning goals. The authors discuss their recent empirical research with 70 college students on the effectiveness of using the structured think-aloud procedure to increase their vocabularies on the Internet. The practical applications of using the structured think-aloud procedure to support students' Internet learning in school or at home are discussed. This includes explaining how teachers can instruct students on critical metacognitive thinking processes by teaching them to use the structured think-aloud procedure. (Contains 3 figures, 2 tables, and 6 resources.)