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Highlights Aligned graphene building blocks take full advantages of the outstanding properties of graphene. Comprehensive review of recent advancements in the utilization of highly aligned graphene aerogels for multifunctional applications. By systematically summarizing the controlled assembly, aligned structural attributes, quantitative characterization methods, anisotropic properties, and multifunctional applications of graphene aerogels, this review enhances understanding of the material's potential for diverse applications, offering tailored properties and novel functionalities.