Iron and steel smelting facilities generate large quantities of airborne particulate matter (PM) through their various activities and production processes. The resulting PM that contains a variety of heavy metals has potentially detrimental impacts on human health and the environment. This study was conducted to assess the potential health effects of the pollution from the heavy metals in the airborne PM sampled in the vicinity of secondary smelting operations in Ile-Ife, Nigeria. X-ray fluorescence (XRF) was used to determine the elemental concentration of Pb, Cr, Cd, Zn, Mn, As, Fe, Cu, and Ni in the size-segregated PM samples. Pollution Indices (PI) consisting of Contamination Factor (CF), Degree of Contamination (DC) and Pollution Index Load (PLI) and Target Hazard Quotient (THQ) were employed to assess the pollution risk associated with the heavy metals in the PM. CF, DC and PLI values were 3< CF <6, >32 and >1, respectively for the three sites, indicating deterioration of the ambient air quality in the vicinity of the smelter. The heavy metals in the airborne PM pose a severe health risk to people living in vicinity of the facility and to its workers. The diminished air quality with the associated health risks directly depends on the industrial emissions from steel production and control measures are recommended to mitigate the likely risks.