<p>This review paper focuses on recent advances in laser-induced graphene (LIG), particularly the spontaneous delamination phenomenon of LIG and its application in fabricating freestanding three-dimensional LIG structures. The fabrication process exploits the detachment of LIG from the substrate due to pyrolysis gas, and it has been experimentally confirmed that delaminated LIG structures, depending on their form, can be applied across a wide range of fields such as energy devices, sensors, antennas, and microrobotics. Based on the latest literature on research related to the LIG delamination phenomenon, this paper analyzes the principles, current development status, and applications of this technology and discusses future directions for its advancement.</p> Graphical abstract <p></p>