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The think-aloud method is a widely used method for evaluating the usability of websites and software. However, it can also be used with cartographic products, an area which has been neglected up to now. It is a method in which test participants verbalise all their thought processes aloud. The participants are given a test scenario containing tasks to be completed. The method aims to reveal the participants’ subjective attitudes toward a product in order to evaluate its usability. The present paper describes the use of the think-aloud method to evaluate the usability of a cartographic work—the regional atlas of the Moravian-Silesian Region. The study includes (I) a complete review of the method, based on the studies conducted; (II) testing tools for working with recorded data; (III) designing an experiment for evaluating the usability of the atlas; and (IV) the resulting qualitative and quantitative evaluation of the atlas based on the obtained results. During the study, three approaches were proposed to process and analyse the audio recordings. The first option was to separate the audio recordings into individual annotations and analyse them. The second option was to convert the recordings to text and perform a linguistic analysis. The third supplementary option was to use all the material produced and to analyse it subjectively and retrospectively, from the researcher’s perspective. All three options were used in the final assessment of the atlas. Based on the participants’ statements, any shortcomings in the studied atlas were identified for each topic (e.g., non-dominant maps or exceedingly complex infographics), and recommendations for their elimination were proposed.

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