High levels of persistent contaminants such as microplastics (MPs) and trace organic compounds (TrOCs) in the aquatic environment have become a major threat on the ecosystem and human health. While MP\'s role as a vector of environmental TrOCs is widely discussed in the literature, the corresponding implications of the interaction between these two compounds on human health (i.e., their joint toxic effect) have not been illustrated. Using a TrOCs model (Triclosan, TCS) and primary MPs (polystyrene microbeads), this work evaluates the sorption and desorption potential of TCS and MPs in simulated environmental and cellular conditions, respectively, and estimates the single and joint toxicity of these interactions toward human cells (Caco-2). Surface functionality of the microbeads highly increased their adsorption capacity of TCS, from 2.3 mg TCS for non-functionalized microbeads to 4.6 mg and 6.1 mg TCS per gram of microbeads for amino- and carboxyl-functionalized MPs, respectively. Using non-functionalized MPs, non-specific \"hydrophobic-like\" interactions and π-π interactions dominated the sorption mechanism of TCS; however, the addition of hydrogen interactions between functionalized microbeads and TCS increased the microbeads\' overall sorption capacity. TCS was desorbed from both functionalized and non-functionalized MPs when changing from environmental conditions to cellular conditions. Desorption was found to be dependent on the matrix complexity and protein content as well as microbead functionality. Finally, toxicity tests suggested that while low concentrations of TCS and MPs (separately) have minor toxic effect toward Caco-2 cells, TCS-sorbed MPs at similar concentrations have an order of magnitude higher toxicity than pristine MPs, potentially associated with the close interaction of both MP and TCS with the cells. Overall, this study not only elucidates the role of MPs as a TrOC vector, but also demonstrates a realistic scenario in which co-presence of these environmental contaminants poses risks to the environment and human health.