Dry weight concentrations of lead in paints on a variety of structures in the urban and suburban environs of a British city (Plymouth, south west England) were determined in situ and ex situ by field-portable X-ray fluorescence spectrometry. Lead was detected in 221 out of 272 analyses, with overall median and mean concentrations of 4180μgg−1 and 29,300μgg−1, respectively, and a maximum concentration of 390,000μgg−1. Highest concentrations were observed in extant paints on poorly maintained, metallic structures, including railings, gates, telephone kiosks and bridges, in various yellow road line paints, and in paints of varying condition on public playground facilities (ramps, climbing frames, monkey bars). Occupants of households in the vicinity of structures that are shedding leaded paint are at potential risk of exposure from paint particles being tracked in on shoes and clothing while children in contact with leaded paints in playgrounds and recreational areas are at potential risk from the direct ingestion of paint flakes. Since the issues highlighted in the present study are neither likely to be restricted to this city, nor to the UK, a greater, general awareness and understanding of the sources and routes of exposure of exterior leaded paint is called for.