A novel fractionation method, based on both particle size and settling characteristics, was employed to examine metal distributions among five fractions. In-stream and stormwater runoff samples were collected from four land use types: highway, urban, agricultural (storm event and irrigation), and natural. Highway samples contained the highest dissolved concentrations for most metals, and freshwater ambient water quality criteria were exceeded for Cd, Cu, Pb, and Zn in the first storm of the water year. Anthropogenic sources were indicated for Cu, Zn, Cd, and Pb in highway and urban samples, and total metal loadings (mg km−2) were observed to be as follows: highway > urban > agricultural storm event ∼ natural > agricultural irrigation. Notably, ∼10-fold higher suspended solids concentration was observed in the agricultural storm event sample, and suspended solids-associated metals were correspondingly elevated. Distribution coefficients revealed the following affinities: Zn, Ni, Cd, and Pb to large dense particles; and Cu, Zn, Cr, Ni, and Pb to colloidal organic matter.