The new millennium has ushered in fresh challenges for educational training of the next generation of workers, global thinkers, and an informed citizenry in a rapidly changing cultural milieu. Methods and tools for exploring phenomena are increasing at rapid rates, especially methods designed to explore how individuals make sense of information and use it to solve problems. Methodological approaches that involve interviewing and probing for human understanding and problem solving have garnered significant attention in the fields of education and psychology. Think-aloud interviews and cognitive laboratory interviews are two related but distinct methodological approaches that can be used to explore human thinking for comprehension and problem solving. However, using these methods to yield accurate, reliable and defensible data to inform key educational goals for business, civics, economics, health, policy, and learning requires careful scrutiny of conditions for their application. For example, the techniques of think-aloud interviews are best applied when probing for processes associated with human problem solving, whereas cognitive laboratory interviews are best applied for human comprehension. In the present book, the two methodological approaches are presented and distinguished, including definitions of goals for application, interview instructions, probing procedures, and interpretation of data for claims about human cognition. Chapters are designed to provide the theoretical and empirical roots for the distinct approaches and examples used to demonstrate practical application. The book is designed to provide an easy-to-read introduction to understanding and practical use of these approaches for uncovering the mysteries of the human information-processing system.