Journey-time exposures to particulate air pollution were investigated in Leicester, UK, between January and March 2005. Samples of TSP, PM10, PM2.5, and PM1 were simultaneously collected using light scattering devices whilst journeys were made by walking an in-car. Over a period of two months, 33 pairs of walking and in-car measurements were collected along two circular routes. Average exposures while walking were seen to be higher than those found in-car for each of the particle fractions: average walking to in-car ratios were 1.2 (± 0.6), 1.5 (± 0.6), 1.3 (± 0.6), and 1.4 (± 0.6) μgm−3 for coarse (TSP–PM10), intermediate (PM10–PM2.5), fine (PM2.5–PM1), and very fine particles (PM1), respectively. Correlations between walking and in-car exposures were seen to be weak for coarse particles (r=0.10, p=0.58), moderate for the intermediate particles (r=0.49, p<0.01) but strong for fine (r=0.89, p<0.01) and very fine (r=0.90, P<0.01) particles. PM10 exposures while walking were on average 70% higher than a nearby roadside fixed-site monitor whilst in-car exposures were 25% higher than the same fixed-site monitor. Particles with an aerodynamic diameter of less than 2.5μm were seen to be highly correlated between walking and in-car particle exposures and a rural fixed-site monitor about 30km south of Leicester.