This study enhances the understanding of the particulate matters (PM2.5 and PM10) and their physical and chemical behavior over the Taj Mahal, Agra, in North-Central India. The mass concentration was determined, and the shape and size of the particles and chemical characterizations have been carried out using SEM–EDX. The high level and significant variation of PM10 (162.2 µg m−3) and PM2.5 (83.9 µg m−3) were observed. The exceedance factor of the present study region is in critical and moderate condition. Morphological characterization reveals the particles of different shapes and sizes, while elemental analysis shows the presence of Si, Al, Fe, Ca, K, Cl, Mg, Na, Cu, and Zn. The dominance of Si indicated the contribution of natural sources, i.e., soil over this region. Three significant sources, viz. soil/road paved dust/vegetative emissions, vehicular/industrial emissions, and intermingling of dust and combustion particles, have been identified using principal component analysis over North-Central India. Health risk analysis of particulate matter identified carcinogenic and non-carcinogenic metals in the present study, which comes in contact with human beings during inhalation. The non-carcinogenic risk was much higher than the acceptable level. The high carcinogenic risks were found in Zn in PM10 and Cu in PM2.5 for both children and adults.