In order to reveal particulate organic carbon (POC) source and mode of transport in the largest river basin on Earth, we sampled the main sediment-laden tributaries of the Amazon system (Solimões, Madeira and Amazon) during two sampling campaigns, following vertical depth-profiles. This sampling technique takes advantage of hydrodynamic sorting to access the full range of solid erosion products transported by the river. Using the Al/Si ratio of the river sediments as a proxy for grain size, we find a general increase in POC content with Al/Si, as sediments become finer. However, the sample set shows marked variability in the POC content for a given Al/Si ratio, with the Madeira River having lower POC content across the measured range in Al/Si. The POC content is not strongly related to the specific surface area (SSA) of the suspended load, and bed sediments have a much lower POC/SSA ratio. These data suggest that SSA exerts a significant, yet partial, control on POC transport in Amazon River suspended sediment. We suggest that the role of clay mineralogy, discrete POC particles and rock-derived POC warrant further attention in order to fully understand POC transport in large rivers.