We report the first ever hourly in situ measurements of speciated organic aerosol composition. Measurements were made during July and August 2004 at Chebogue Point, Nova Scotia, using a novel thermal desorption aerosol GC/MS-FID (TAG) instrument as part of the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT). Hourly time resolution measurements of organic marker compounds were used to define several different source types contributing to the aerosols observed, including two aged anthropogenic sources from the United States, oxidized biogenic aerosols from Maine and Canada, local biogenic contributions to secondary organic aerosol (SOA), local anthropogenic contributions to hydrocarbon-like organic aerosol (HOA), and a potential marine or dairy source. These TAG-defined sources were used to separate aerosol mass spectrometer (AMS) measurements of total organics, SO42−, NO3−, and NH4+, along with total aerosol black carbon (BC) into several distinct particle types. Average organic aerosol mass ranged from 33% of the total aerosol mass during anthropogenic U.S. outflow events to 81% of total aerosol mass during biogenic oxidation events arriving from Maine and Canada during 26 July to 15 August 2004.