Methods of wet and dry crushing are adopted to experiment on spent lithium-ion batteries in this investigation. Particle size distribution is analyzed using the wet and dry screening respectively and fine crushed products are characterized by XRD, SEM and EDX. A comprehensive comparison of the characteristics between the two crushing methods indicates that the wet crushing results in an enrichment of each component in spent lithium-ion batteries to fine fractions because of the scouring action of water flow, which makes the fine products complicated and lost; while the dry crushing method can bring the selective crushing characteristics of spent lithium-ion batteries into full play, and in this case, lithium cobalt oxide and graphite electrode materials can be liberated from aluminum foil and copper foil without the overcrushing of the other components in spent lithium-ion batteries. Thus, the purity and dispersion of electrode materials can be improved to create favorable conditions for subsequent purification and regeneration.