Origami offers two-dimensional (2D) materials with great potential for applications in flexible electronics, sensors, and smart devices. However, the dynamic process, which is crucial to construct origami, is too fast to be characterized by using state-of-the-art experimental techniques. Here, to understand the dynamics and kinetics at the atomic level, we explore the edge effects, structural and energy evolution during the origami process of an elliptical graphene nano-island (GNI) on a highly ordered pyrolytic graphite (HOPG) substrate by employing steered molecular dynamics simulations. The results reveal that a sharper armchair edge is much easier to be lifted up and realize origami than a blunt zigzag edge. The potential energy of the GNI increases at the lifting-up stage, reaches the maximum at the beginning of the bending stage, decreases as the formation of van der Waals overlap, and finally reaches an energy minimum at a half-folded configuration. The unfolding barriers of elliptical GNIs with different lengths of major axis show that the major axis should be larger than 242 Å to achieve a stable single-folded structure at room temperature. These findings pave the way for pursuing other 2D material origami and preparing for origami-based nanodevices.