Exposure to ambient particulate matter (PM) is statistically significantly associated with morbidity and mortality. The objectives of this study were (a) to investigate in vivo pulmonary and systemic cytotoxicity and inflammatory activity in compromised animals exposed to PM and (b) to investigate the relationships of the outcomes to the chemical compositions of particular polycyclic aromatic hydrocarbons (PAH) and transition metals in the PM. The PM samples were collected in European cities representing contrasting situations. Exposure of spontaneously hypertensive rats (7 mg of PM/kg) resulted in pulmonary inflammation, cellular toxicity and the induction of blood fibrinogen. Coarse PM generally caused stronger effects per mg than fine particles. Positive correlations between lactate dehydrogenase, proteins, and some inflammation parameters and the particle metal and PAH content were found. PM rich in PAH also led to increased blood fibrinogen. Removal of particles but not the organics (i.e., PAH) of a sample led to reduced inflammation in the lungs. The present study highlights the importance of metals as well as PM-bound PAH in particle biological outcomes. It supports the hypothesis that, on an equal mass basis, particle health effects differ due to differences in compositions and size.