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We describe our efforts to compare data collection methods using two think-aloud protocols in preparation to be used as a basis for automatic structuring and labeling of a large database of high-dimensional human activities data into a valuable resource for research in cognitive robotics. The envisioned dataset, currently in development, will contain synchronously recorded multimodal data, including audio, video, and biosignals (eye-tracking, motion-tracking, muscle and brain activity) from about 100 participants performing everyday activities while describing their task through use of think-aloud protocols. This paper provides details of our pilot recordings in the well-established and scalable “table setting scenario,” describes the concurrent and retrospective think-aloud protocols used, the methods used to analyze them, and compares their potential impact on the data collected as well as the automatic data segmentation and structuring process.