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The brick-and-mortar structure inspired by nature, such as in nacre, is considered one of the most optimal designs for structural composites. Given the large number of design possibilities, extensive computational work is required to guide their manufacturing. Here, we propose a computational framework that combines statistical analysis and machine learning with finite element analysis to establish structure–property design strategies for brick-and-mortar composites. Approximately 20,000 models with different geometrical designs were categorized into good and bad based on their failure modes, with statistical analysis of the results used to find the importance of each feature. Aspect ratio of the bricks and horizontal mortar thickness were identified as the main influencing features. A decision tree machine learning model was then established to draw the boundaries of good design space. This approach might be …