Large-scale gridded population product datasets have become crucial sources of information for sustainable development initiatives. However, mainstream modeling approaches (e.g., dasymetric mapping based on Multiple Linear Regression or Random Forest Regression) do not consider the heterogeneity and multiscale characteristics of the spatial relationships between influencing factors and populations, which may seriously degrade the accuracy of the prediction results in some areas. This issue may be even more severe in large-scale gridded population products. Furthermore, the lack of detailed 3D human settlement data likewise poses a significant challenge to the accuracy of these data products. The emergence of the unprecedented Global Human Settlement Layer (GHSL) data package offers a possible solution to this long-standing challenge. Therefore, this study proposes a new Gridded Population Mapping (GPM) method that utilizes the Multiscale Geographically Weighted Regression (MGWR) model in conjunction with GHSL-3D Building, POI, nighttime light, and land use/cover datasets to disaggregate population data for third-level administrative units (districts and counties) in mainland China into 100 m grid cells. Compared to the WorldPop product, the new population map reduces the mean absolute error at the fourth-level administrative units (townships and streets) by 35%, 51%, and 13% in three test regions. The proposed mapping approach is poised to become a crucial reference for generating next-generation global demographic maps.