Angularly resolved elastic light scattering patterns from individual atmospheric aerosol particles (diameter 0.5–12 micrometers) sampled during fall (October 2004) at an urban site in the Baltimore-Washington metroplex are reported. These two-dimensional angular optical scattering (TAOS) patterns were collected for polar scattering angles θ varying from approximately 75° to 135° and azimuthal angles ϕ varying from 0° to 360°. Approximately 6000 scattering patterns were sampled over a span of 18 hours from an inlet located above our laboratory roof at Adelphi, Maryland. Our instrument recorded light scattering patterns of higher resolution and accuracy than have previously been achievable. The patterns suggest that background aerosol particles have diverse morphologies ranging from single spheres to complex structures. The frequency of occurrence of particle morphologies inferred from the TAOS patterns is strongly dependent on size. For nominally 1-μm particles, 65% appear spherical (or perturbed sphere) and only about 9% have complex structure (as suggested by their complex scattering features); whereas for nominally 5-μm particles, only 5% appear spherical (or perturbed sphere) and 71% appear to have complex structure. The patterns are quantitatively characterized using a degree of symmetry (Dsym) factor, calculated by examining both mirror and rotational symmetries in each pattern. In our measurements, atmospheric particles have two distinct populations: mostly micron-sized particles with Dsym values close to that of spheres and a population of mostly supermicron particles having a low but broad range of Dsym values. These observations are consistent with the commonly accepted notion that most micron-sized particles (in the accumulation mode) appear to be nearly spherical and are probably formed in the atmosphere through gas-particle reactions; whereas most supermicron particles appear to be nonspherical and are likely directly injected into the atmosphere. Our observations suggest that Lorenz-Mie theory may be adequate for most micron-sized particles but not for supermicron particles.