This review provides a comprehensive overview of highly aligned graphene aerogels and their multifunctional applications. It highlights the fabrication methods, controlled assembly, aligned structural attributes, quantitative characterization methods, anisotropic properties, and multifunctional applications of these materials. The unique combination of aligned structure, high surface area, excellent electrical conductivity, mechanical stability, thermal conductivity, and porous nature of highly aligned graphene aerogels allows for tailored and enhanced performance in specific directions, enabling advancements in diverse fields such as electronics, environmental applications, thermal management, and energy storage. The review discusses the challenges and potential opportunities in this fast-growing research area, aiming to contribute to broader understanding and utilization of highly aligned graphene aerogels as multifunctional materials with tailored properties and novel functionalities.This review provides a comprehensive overview of highly aligned graphene aerogels and their multifunctional applications. It highlights the fabrication methods, controlled assembly, aligned structural attributes, quantitative characterization methods, anisotropic properties, and multifunctional applications of these materials. The unique combination of aligned structure, high surface area, excellent electrical conductivity, mechanical stability, thermal conductivity, and porous nature of highly aligned graphene aerogels allows for tailored and enhanced performance in specific directions, enabling advancements in diverse fields such as electronics, environmental applications, thermal management, and energy storage. The review discusses the challenges and potential opportunities in this fast-growing research area, aiming to contribute to broader understanding and utilization of highly aligned graphene aerogels as multifunctional materials with tailored properties and novel functionalities.