Inspired by nature, materials scientists have been exploring and designing various biomimetic materials. Among them, composite materials with brick-and-mortar-like structure synthesized from organic and inorganic materials (BMOIs) have attracted increasing attention from scholars. These materials have the advantages of high strength, excellent flame retardancy, and good designability, which can meet the requirements of various fields for materials and have extremely high research value. Despite the increasing interest in and applications of this type of structural material, there is still a dearth of comprehensive reviews, leaving the scientific community with a limited understanding of its properties and applications. In this paper, we review the preparation, interface interaction, and research progress of BMOIs, and propose possible future development directions for this class of materials.