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Summary The Orientale Basin is the youngest and best-preserved multi-ring impact basin on the Moon. It is approximately 930 km in diameter and comprises three concentric rings—the Cordillera, Inner Rook, and Outer Rook rings. We used Gravity Recovery and Interior Laboratory (GRAIL) mission gravity data (GRGM1200B, truncated to degree 660) to invert the three-dimensional (3D) density structure associated with the basin’s mascon and ring-related crustal anomalies. To separate longer and shorter-wavelength signals, we performed inversions using (1) spherical harmonic degrees 2–660 to characterise the basin’s deep structure and (2) degrees 60–660 to highlight crustal-scale heterogeneity. The inversion with degree and order of 2–660 resolves a basin-wide central positive density anomaly beneath the inner depression, extending from a depth of ∼16–80 km, corresponding to uplifted mantle. This anomaly persists below the crust–mantle boundary; however, its deep continuation should be interpreted cautiously because it may partially reflect vertical smearing in the gravity inversion. Nonetheless, the spatial association of this anomaly with a mascon rooted in the upper mantle is compatible with impact-driven uplift of dense material from depth, followed by post-impact thermal evolution and relaxation processes. The inversion with degree and order of 60–660 indicates alternating positive and negative density anomalies associated with the ring system. Prominent ring-parallel positive anomalies occur along the Outer Rook Ring and Cordillera Ring, extending to ∼30–35 km depth and exhibiting a density contrast of ∼60–200 kg/m3. The geometry and lateral continuity of these anomalies across multiple rings support an interpretation of ring-controlled crustal heterogeneity, consistent with either intrusion and structurally focused modification along ring-related discontinuities or impact-generated fracturing that provided pathways for magma ascent. The results of this study provide quantitative constraints on the depth, magnitude, and spatial distribution of density anomalies associated with the Orientale mascon and ring system, thereby improving the subsurface framework for regional geological interpretation and supporting future lunar landing-site geophysical investigations and in situ sampling. Based on the inferred crustal density architecture, we propose that future geophysical sampling efforts should prioritise the Outer Rook Ring and Cordillera Ring, where the observed ring-parallel anomalies may provide insights into crustal modification processes and the composition of the lunar interior.