As rarely large flake graphite (9 mesh) was recently exploited in China, it was innovatively developed as the raw material to prepare a novel wound dressing based on large expanded graphite (EG) in this work. The EG worms were prepared in an easy oxidative intercalation and thermal expansion method. Afterward, chitosan was grafted onto the surface of EG by chemical modification, forming CS-EG worms. CS-EG sponge dressings were then obtained by pressing a number of CS-EG worms together by external force. Due to the porous structure and large specific surface area, the produced CS-EG sponges exhibited outstanding adsorption capacity for wound exudate. They could also promote blood coagulation by adsorbing the blood cells and proteins quickly and effectively, showing excellent hemostatic performance. The eminent performances and the simple preparation process ensure the great application potential of CS-EG as a dressing material. This is also the first time to report the application of the traditional carbon material, EG, to act as a dressing material after chemical modification.