increases with primary OA (POA) as does the nitrogen-tocarbon (N/C, ∼0.02). Ambient organic-mass-to-organic-carbon ratios (OM/OC) are directly quantified and correlate well with O/C (R2 ) 0.997) for ambient OA because of low N/C. Ambient O/C and OM/OC have values consistent with those recently reported from other techniques. Positive matrix factorization applied to ambient OA identifies factors with distinct O/C and OM/OC trends. The highest O/C and OM/OC (1.0 and 2.5, respectively) are observed for aged ambient oxygenated OA, significantly exceeding values for traditional chamberSOA,whilelaboratory-producedprimarybiomassburning OA (BBOA) is similar to ambient BBOA, O/C of 0.3–0.4. Hydrocarbon-like OA (HOA), a surrogate for urban combustion POA, has the lowest O/C (0.06–0.10), similar to vehicle exhaust. An approximation for predicting O/C from unit mass resolution data is also presented.