Population spatialization reveals the distribution and quantity of the population in geographic space with gridded population maps. Fine-scale population spatialization is essential for urbanization and disaster prevention. Previous approaches have used remotely sensed imagery to disaggregate census data, but this approach has limitations. For example, large-scale population censuses cannot be conducted in underdeveloped countries or regions, and remote sensing data lack semantic information indicating the different human activities occurring in a precise geographic location. Geospatial big data and machine learning provide new fine-scale population distribution mapping methods. In this paper, 30 features are extracted using easily accessible multisource geographic data. Then, a building-scale population estimation model is trained by a random forest (RF) regression algorithm. The results show that 91% of the buildings in Lin’an District have absolute error values of less than six compared with the actual population data. In a comparison with a multiple linear (ML) regression model, the mean absolute errors of the RF and ML models are 2.52 and 3.21, respectively, the root mean squared errors are 8.2 and 9.8, and the R² values are 0.44 and 0.18. The RF model performs better at building-scale population estimation using easily accessible multisource geographic data. Future work will improve the model accuracy in densely populated areas.