Mineral dust particles in the lower atmosphere may significantly influence radiative and optical budgets, along with the net chemical balance, through their interactions with ambient chemicals. Their ability to absorb/scatter incoming radiation strongly depends on their chemical composition (i.e., distribution of major crustal elements), but as yet there is no adequate regional database with regard to this for the Indian region. To create a regional database of background mineral dust from a semi-arid zone of western India, we measured the chemical composition of ambient particles (with aerodynamic diameter ≤ 5 µm; PM5), collected from seven locations of Jaipur city (in the vicinity of Thar Desert; Rajasthan) at varying altitudes, during late-winter of 2012. The chemical compositions of the sampled particles at both bulk and individual levels were measured using X-ray fluorescence (XRF) and Scanning Electron Microscope equipped with Energy Dispersive X-ray (SEM-EDX) techniques, respectively. Significant differences in chemical compositions were observed among the seven sites, yet the bulk chemical compositions of the particles were broadly consistent with those of individual particles. Average elemental ratios of Mg/Al, Si/Al, K/Al, Ca/Al, Mn/Al, Fe/Al were found to be 0.44 ± 0.22, 1.96 ± 0.90, 0.65 ± 0.22, 1.52 ± 0.40, 0.84 and 1.54 ± 1.67 respectively. We also estimated the complex refractive index (RIs at 550 nm wavelength) for the studied sites, yielding an average n and k (the real and imaginary parts of RI, respectively) of (1.56 ± 0.03) + (6.5 ± 4.6) × 10–3i, with the aerosols collected from Kukas Hill area (27.02°N, 75.85°E) having the highest iron (Fe) mass fraction (~43%). Non-crustal elements e.g., Cu, S, C, Ag and Pb were found only in aerosols over the main city Birla Temple (Jaipur) at ground level (26.89°N, 75.81°E).