Untargeted data analyses were performed using comprehensive GCxGC-ToF/MS measurements. Univariate and multivariate chemometric tools, such as analysis of variance (ANOVA), principal component analysis (PCA), and ANOVA simultaneous component analysis (ASCA), were used to reduce the data to highly significant and specific fea- tures. In addition fast and accurate automated compound classification algorithms were developed for initial data screening. This study reveals substances not previously considered in the literature as meaningful markers for aerosol sources and provides valuable input for the establishment of an effect/cause relationship between aerosols and the adverse effects induced in human health.