The Nectarian-aged Crisium basin exhibits an extremely thin crust and complicated lunar geological history. This large multi-ring impact basin is characterized by prolonged lunar volcanism ranging from the Imbrian age to the Eratosthenian period, forming the high-Ti mare unit, low-Ti mare basalts, and very low-Ti mare unit. We produced an updated geological map of the Crisium basin and defined four mare units (Im1: 3.74 Ga; Im2: 3.49 Ga; Im3: 3.56 Ga; EIm: 2.49 Ga) in terms of distinct composition and mineralogy. Olivine was widely determined in the Ti-rich Im1, implying the hybridization source in the lunar mantle with the occurrence of small-scale convective overturn. The major phase of low-Ti basaltic volcanism occurred c.a. 3.5 Ga, forming Im2 and Im3 in the western area. The youngest mare unit (EIm) has slight variations of pyroxene compositions, implying a decrease of calcic content of basaltic volcanisms with time. Later, distal material transports from large impact events in highlands could complicate the mixing of local mare basalts in the Copernicus age, especially the Im3 unit. The identified olivine-bearing outcrops and widely Mg-rich materials (Mg# > 70, where Mg# = molar 100 × Mg/(Mg + Fe)) in the western highlands, assumed to be the occurrence of the Mg-suite candidates, require future lunar exploration missions to validate.