Particulate and vapor concentrations of atmospheric As have been measured over various marine and continental areas. Particulate sample were collected on double Whatman 41 filters. Particulate-vapor samples were collected using an in-line filter system with a 0.45-μm pore size Nuclepore filters as a particle prefilter in front of two Whatman 41 filters impregnated with tetrabutylammonium hydroxide and glycerol for vapor As collection. Arsenic determinations were by destructive neutron activation. The data from the Nuclepore-impregnated filter samples indicates that the major fraction of AS in the atmosphere is particulate but a vapor component of As is detectable, most frequently associated with high sampling temperatures and high total As concentrations. With the data presented here, estimates of representative global near-surface concentrations of atmospheric arsenic have been made.