Abstract: Potassium-rich brine in the Sichuan Basin has been much studied in recent years, but few studies have focused on the distribution and migration of salt basin and the differences of potassium formation mechanisms. This work examined the salt-gathering and potassium formation of potassium-rich brine during the Triassic in the Sichuan Basin using lithofacies palaeogeographic depiction and geochemical analyses. (1) The favorable sedimentary facies controlling the formation of potassium-rich brine during the Triassic in the Sichuan Basin are evaporation platform and restricted platform, whereas the salt basin is one of the main factors controlling the poly-salt center. (2) The distribution and migration of this salt basin were affected by certain factors. The salt basin of the Jialingjiang Formation was mainly distributed in the east and central Sichuan Basin, whereas that of the Leikoupo Formation was mainly distributed in the central and west Sichuan Basin. The sedimentary centers have gradually moved westward and become smaller. (3) Three main formation mechanisms were identified for the potassium-rich brine during the Triassic in the Sichuan Basin, i.e., evaporation and concentration of seawater, surface fresh water leaching, and deep water-rock reaction. Fresh water leaching was characterized by low anomaly δ18O and δ13C values. Water-rock reaction was mainly related to temperature, and high temperature environment (caused by burial depth, overthrust and deep hydrothermal fluids) was beneficial to water-rock reaction. The characteristics of water-rock reaction do not correspond to the increase ratio of K·103/Cl and Br·103/Cl in brine, and the Rb+ content of the brine was high. (4) The formation mechanisms of potassium-rich brine differed between different areas of the Sichuan Basin. In east Sichuan, the evaporation and concentration of seawater, together with meteoric fresh water leaching, was the main formation factor, whereas the evaporation and concentration of seawater and water–rock reaction predominated in west Sichuan. This study of the sedimentary environment and formation mechanisms is of significance to the exploration and exploitation of potassium-rich brine in the Sichuan Basin.