A time series of organic carbon export from Gulf of Maine (GoM) watersheds was compared to a time series of biological, chemical, bio-optical, and hydrographic properties, measured across the GoM between Yarmouth, NS, Canada, and Portland, ME, U.S. Optical proxies were used to quantify the dissolved organic carbon (DOC) and particulate organic carbon in the GoM. The Load Estimator regression model applied to river discharge data demonstrated that riverine DOC export (and its decadal variance) has increased over the last 80 years. Several extraordinarily wet years (2006–2010) resulted in a massive pulse of chromophoric dissolved organic matter (CDOM; proxy for DOC) into the western GoM along with unidentified optically scattering material (<0.2 μm diameter). A survey of DOC in the GoM and Scotian Shelf showed the strong influence of the Gulf of Saint Lawrence on the DOC that enters the GoM. A deep plume of CDOM-rich water was observed near the coast of Maine which decreased in concentration eastward. The Forel-Ule color scale was derived and compared to the same measurements made in 1912–1913 by Henry Bigelow. Results show that the GoM has yellowed in the last century, particularly in the region of the extension of the Eastern Maine Coastal Current. Time lags between DOC discharge and its appearance in the GoM increased with distance from the river mouths. Algae were also a significant source of DOC but not CDOM. Gulf-wide algal primary production has decreased. Increases in precipitation and DOC discharge to the GoM are predicted over the next century.