Airborne particles in the environment are generally smaller than a couple of microns. Use of magnetic force to collect aerosol particles thus has not been popular as the other means. There are billions of airborne particles emitted by a host of man-made sources with the particle size smaller than 1 mu m and possess some magnetic susceptibility. We are thus interested in the use of high-gradient magnetic collection to extract the magnetic fraction in an aerosol population. In this study, we reported that the magnetic force is the dominant force in collection of ferromagnetic particles of mobility equivalent size larger than or equal to 50 nm in a high-gradient permanent-magnetic aerosol collector, while the diffusiophoretic force is responsible for particles smaller than 10 nm. Both forces compete for particles in between these two sizes in the magnetic aerosol collector designed for this study. To enable a wide-range effective collection of aerosol particles across entire size spectrum from a few nanometers to tens of a micron, the ORNL-designed high-gradient magnetic collector would require the use of an engineered matrix. Thus, the matrix design for a specific application becomes application specific. Irrespective of the collection efficiency, the use of permanent magnets to collect magnetic particles is feasible and also highly selective because it tunes into the magnetic susceptibility of the particles as well as the size. Lastly, the use of permanent magnets enables the collector to be operated at a minimal power requirement, which is a critical factor in long-term field operation.