This study evaluates the use of magnetic susceptibility and magnetic parameter measurements in assessing spatial and temporal variations of pollutants that emanated from mining industries in and around Sudbury, Ontario, Canada. For this purpose, in situ magnetic susceptibility (κin situ) was measured at 106 sites on a grid of 10 km × 10 km and 5 km × 5 km. The κin situ values ranged from 2 × 10−5 to 149 × 10−5 SI, and the highest κin situ values were observed near the active (Copper Cliff) and inactive (Coniston) mining sites. The lowest κin situ values were measured at increased distances from possible pollution sources; therefore, mapping of in situ magnetic susceptibility values is a proxy to polluted areas in and around Sudbury. To evaluate potential anthropogenic and (or) lithogenic input to κin situ, low-frequency mass specific magnetic susceptibility (χlf) variations with depth were classified into four different types of profiles. For further investigation of magnetic minerals in the samples, laboratory measurements of magnetic susceptibility, frequency dependence of magnetic susceptibility, hysteresis properties, thermosusceptibility curves, anhysteretic and isothermal magnetizations, and scanning electron microscopy – energy-dispersive X-ray spectroscopy (SEM–EDS) were also conducted on the soil samples. Laboratory measurements indicated that ferrimagnetic minerals (e.g., magnetite) of variable grain size were the dominant magnetic minerals, with the exception of one site that contained an iron sulfide (greigite) phase near a mine waste site. Magnetic spherules observed in SEM micrographs are of variable sizes (6–60 μm), suggesting that suspended particulate matter (PM10) is present, and may be a health concern. At some sites, EDS analysis showed that heavy metals (Co, Al, and Ni), which threaten human health, are also present in the study area.