Pollution exhibits significant variations horizontally and vertically within cities; therefore, the size and three-dimensional (3D) spatial distribution of population are significant determinants of urban health. This paper presents a novel methodology, 3D digital geography (3DIG) methodology, for investigating 3D spatial distributions of population in close proximity to traffic, thus the potential highly exposed population under traffic impacts. 3DIG applies geographic information system and fine-resolution (5 m) digital terrain models to obtain the number of building floors in residential zones of the Taipei metropolis; the vertical distribution of population at different floors was estimated based on demographic data in each census tract. In addition, population within 5, 10, 20, 50, and 100 m from the roadways was estimated. Field validation indicated that model results were reliable and accurate; the final population estimation differs only by 0.88% from the demographic database. The results showed that among the total 6.5 million Taipei residents, 0.8 (12.3%), 1.5 (22.9%), 2.3 (34.9), and 2.7 (41.1%) million residents live on the first or second floor within 5, 10, 20, and 50 m, respectively, of municipal roads. There are 22 census tracts with more than half of their residents living on the first or second floor within 5 m of municipal roads. In addition, half of the towns in Taipei city and county with >13.9% and 12.1% of residents live on the first and second floors within 5 m of municipal roads, respectively. These findings highlight the huge number of Taipei residents in close proximity to traffic and have significant implications for exposure assessment and environmental epidemiological studies. This study demonstrates that 3DIG is a versatile methodology for various research and policy planning in which 3D spatial population distribution is the central focus.