Particle surface area has recently been considered as a possible metric in an attempt to correlate particle characteristics with health effects. In order to provide input to such studies, two Nanoparticle Surface Area Monitors (NSAMs, TSI, Inc.) were deployed in different urban sites within Los Angeles to measure the concentration levels and the diurnal profiles of the surface area of ambient particles. The NSAM's principle of operation is based on the unipolar diffusion charging of particles. Results show that the particle surface concentration decreases from ∼150 µm 2 cm −3 next to a freeway to ∼100 µm 2 cm −3 at 100 m downwind of the freeway, and levels decline to 50-70 µm 2 cm −3 at urban background sites. Up to 51% and 30% of the total surface area corresponded to particles <40 nm next to the freeway and at an urban background site, respectively. The NSAM signal was well correlated with a reconstructed surface concentration based on the particle number size distribution measured with collocated Scanning Mobility Particle Sizers (SMPSs, TSI, Inc.). In addition, the mean surface diameter calculated by combination of the NSAM and the total particle number concentration measured by a Condensation Particle Counter (CPC, TSI, Inc.) was in reasonable agreement with the arithmetic mean SMPS diameter, especially at the urban site. This study corroborates earlier findings on the application of diffusion chargers for ambient particle monitoring by demonstrating that they can be effectively used to monitor the particle surface concentration, or Received 24 June 2006; accepted 9 February 2007. This research was supported by the Southern California Particle Center (SCPC), funded by EPA under the STAR program through Grant RD-8324-1301-0 to the University of Southern California and was also supported by the NIEHS-NIH grant no. ES-12243 and the California Air Resources Board (CARB) contract no. 03-329. We would also like to thank Dr. Manisha Singh (TSI Inc.) for availing the NSAM monitors and her assistance with the operation of these instruments. The research described herein has not been subjected to the EPA required peer and policy review and therefore does not necessarily reflect the views of the agency, and no official endorsement should be inferred. Mention of trade names or commercial products does not constitute an endorsement or recommendation for use.Address correspondence to Constantinos Sioutas, University of Southern California, Department of Civil and Environmental Engineering, 3620 S. Vermont Avenue, Los Angeles, CA 90089, USA. E-mail: sioutas@usc.edu combined with a CPC to derive the mean surface diameter with high temporal resolution.