Reliable, inexpensive, environment-friendly, and durable properties of carbon materials with unique and outstanding photoelectric performance is highly desired for myriad of applications such as catalysis and energy storage. Since lattice modulation is a vital method of surface modification of materials, which form by an external force during the synthesis process, causing the internal compression and stretching, leading to lattice sliding event. In this review, we present a summary of different methods to tailor the lattice modulation in 2D carbon-based materials, including grain/twin boundary, lattice strain, lattice distortion, and lattice defects. This overview highlights the implication control of the diverse morphologies of nanocrystals and how to tailor the materials properties without adding any polymers. The improvement in the performance of 2D carbon materials ranges from the enhancement of charge transport and conductivity, structural stability, high-performance of light absorption capacity, and efficient selectivity promote the future prospect of 2D carbon materials broaden their applications in terms of energy conversion and storage. Finally, some perspectives are proposed on the future developments and challenges on 2D carbon materials towards energy storage applications.