The preparation of graphene from graphite is critical for both theoretical studies and real-world applications. Herein, we present a systematic study to explore the fundamental factors that control the exfoliation of graphite into graphene in a salt-intercalation exfoliation system, using various inorganic salts as intercalators. The yields of the thin graphene sheets obtained, measured via UV-vis absorption spectrophotometry, suggest that both cations and anions significantly influence the exfoliation yields. Xray photoelectron spectroscopy and energy dispersive spectroscopy analysis showed that both anions and cations become inserted into the space between conjugated graphite layers during the intercalation process. X-ray diffraction spectra revealed that the anion can enhance the salt-intercalation exfoliation by expanding the interlayer spacing. Compared to lithium chloride, both potassium chloride and lithium sulfate can significantly enhance the exfoliation yields of graphene. Optimizing the cation and anion species can improve the yield of graphene, because co-intercalation with both anions and cations occurs during the intercalation process in the solution of inorganic salts. Our work provides a guide for rationally designing the salt-intercalation exfoliation procedure to obtain higher yields of exfoliated 2D materials.