We present results from the Global Change Expedition/ Coordinated Air‐Sea Experiment/Western Atlantic Ocean Experiment (GCE/CASE/WATOX) research cruise conducted from July to September 1988 in the North Atlantic Ocean aboard the NOAA shipMt. Mitchell. We examine the correlations between measurements of aerosol black carbon (BC, a tracer for combustion emissions), radon 222 (Rn, a tracer for natural emissions from land masses), and calculated isentropic back trajectories from the ship's position during two portions of the cruise that circled the North Atlantic Ocean. The results suggest four distinct categories of origin of the sampled air mass, with trajectories connecting back to different geographical areas: case A, trajectories from inhabited land, with the air mass containing strongly correlated BC and Rn; case B, trajectories from uninhabited (far northern) land, with Rn but little BC; case C, contaminated marine air, with little Rn but moderate BC, correlated with observations of combustion sources (other ships, etc.) in the vicinity; and case D, air masses of remote marine origin, with low BC and low Rn content. The requirements of the trajectory analyses lead to an improved understanding of the transport pathways across the ocean. We conclude that real‐time measurements of aerosol black carbon and radon, coupled with timely meteorological analyses, can be a powerful indicator of air mass origin both retrospectively and during the course of an experiment to assist in the scheduling of other measurements.