This dataset describes a series of aerosol and meteorological measurements collected in the Great Barrier Reef (GBR) Marine Park collected during the "GBR as a significant source of climatically relevant aerosol particles" campaign, known as "Reef to Rainforest" (R2R). The data covers a broad area of the GBR marine park (-27.3091 to -16.95169 latitudinally, 145.9705 to 154.1146 longitudinally) over approximately one month, from 28th September, 2016 to 24th October, 2016. The data was collected at two sites – one aboard the Australian Government Research Vessel Investigator (RVI), and an onshore site at Garner's Beach, QLD, Australia (-17.8222S, 146.1023E). Parameters measured include particle size distribution, number concentration, composition cloud condensation nuclei (CCN) properties, concentrations of gases and markers including black carbon, radon, carbon monoxide, carbon dioxide, volatile organic compounds (VOCs), dimethylsulfide (DMS), upper air particle concentration/composition, cloud or low lying fog presence, cloud top height, depolarisation ratio, aerosol scattering and optical thickness. The observations were collected in the hope of improving our understanding of the local climate and aerosol properties, which in turn will improve local models and better inform regulatory bodies protecting the GBR.