High-alumina (HA) mare basalts play a critical role in lunar mantle differentiation. Although remote sensing methods have speculated their potential presence regions based on sample FeO and TiO2 compositions, the location and distribution characteristics of HA basalts have not been provided. In this study, the compositions of exposed rocks in Mare Imbrium were determined using Lunar Reconnaissance Orbiter (LRO) Diviner oxides and Lunar Prospector Gamma-Ray Spectrometer (LP-GRS) Thorium (Th) products. The exposed HA basalts were identified based on laboratory lithology classification criteria and Al2O3 abundance. The HA basalt units were mapped based on lunar topographic data, and their morphological geological characteristics were calculated based on elevation data. The results show that there are 8406 HA basalt pixels and 17 original units formed by volcanic eruptions in Mare Imbrium. The statistics of their morphology characteristics show that the HA basalts are widely distributed in the northern part of Mare Imbrium, and their compositions have a large range of variation. These units have different area and volume, and the layers formed were discontinuous. The characteristic analysis shows that the aluminum-bearing volcanic activities in Mare Imbrium were irregular. The eruptions of four different source regions occurred in three phases, and the scale and extent of the eruptions were different. The results in this study provide reliable evidence for the heterogeneity of the lunar mantle and contribute valuable information to the formation process of early lunar mantle materials.