The heteroaggregation of engineered nanoparticles (ENPs) with naturally occurring colloids (NOCs) plays an important role in determining the ultimate fate and transport of nanomaterials in the environment. The objective of this research was to characterize the potential for heteroaggregation between functionalized multiwall carbon nanotubes (MWCNTs) with NOCs in the aquatic environment. Carboxylated MWCNTs (COOH-MWCNTs) and amine functionalized MWCNTs (NH2-MWCNTs) were studied. The natural clay kaolinite was chosen as a model NOC due to its widespread presence in the natural environment and unique charge heterogeneity. In this study, the aggregation between CNTs and kaolinite was analyzed for a range of CNT:NOC ratios and pH as well as in different source waters in a series of sedimentation and aggregation experiments. Sedimentation was monitored using ultraviolet-visible (UV-VIS) spectroscopy, while aggregation was characterized by dynamic light scattering. The heteroaggregation of the COOH-MWCNTs was found to be heavily dependent on pH and the CNT:NOC ratio. The sedimentation rate of the CNT-NOC mixture indicated by UV-VIS spectroscopy and average particle size measured by DLS both increased at low pH while the CNT solution remained stable over time when tested at the same solution chemistry. As the CNT:NOC ratio decreased, the CNT-NOC mixture demonstrated enhanced sedimentation behavior at pH 3. The enhanced sedimentation coupled with increasing particle size of the mixture indicated the presence of CNT-NOC heteroaggregates. At higher pH, no enhanced sedimentation occurred for the range of ratios tested. The NH2-MWCNTs were not dispersible at neutral pH were therefore only tested at pH 3. All solutions regardless of ratio indicated no significant evidence of enhanced sedimentation due to heteroaggregation for the NH2-MWCNTs in this study. Filtered and unfiltered natural water samples from Lake Houston and the Trinity River were also analyzed and found to significantly enhance the sedimentation of the CNTs at neutral pH. The unfiltered samples exhibited enhanced sedimentation of the COOH-MWCNTs compared to the filtered samples. There was also evidence of enhanced removal of other particles present in the natural water sample due to the addition of CNTs. This indicates that the presence of CNTs could affect the transport of other contaminants in aquatic systems, altering the distribution of contaminants particularly at the sediment-water interface. These results suggest that NOCs enhance the sedimentation of CNTs in the natural environment and are highly dependent on pH and the ratio of carbon nanotube to natural colloid.