This study examined the effects of micro- (crystallinity) and macro (orientation)-crystalline properties of graphite on the initial efficiency, discharge capacity, and rate performance of anodic materials. Needle coke and regular coke were selected as raw materials and pulverized to 2–25 μm to determine the effects of crystalline properties on particle shape after pulverization. Needle coke with outstanding crystallinity had high initial efficiency, and smaller particles with larger specific surface areas saw increased irreversible capacity due to the formation of SEI layers. Because of cavities existing between crystals, the poorer the crystalline properties were, the greater the capacity of the lithium ions increased. As such, regular coke had a 30 mAh/g higher discharge capacity than that of needle coke. Rate performance was more affected by particle size than by crystalline structure, and was the highest at a particle distribution of 10–15 μm.