Exploring the adsorption of organic compounds onto microplastics (MPs) is of great significance for understanding their environmental fate and evaluating their ecological risks. To date, various techniques, e.g., experiments, simulations, and prediction models, have been utilized for exploring the adsorption of different organic compounds onto MPs. In this review, we systematically introduce the sources of MPs, the interactions between MPs and organic compounds, the factors influencing the adsorption of organic compounds onto MPs, and research advances in investigating the adsorption of organic compounds by microplastics with different techniques. We also point out that the structures of MPs and environmental factors can have distinct effects on the adsorption mechanisms, and the adsorption mechanisms for numerous organic compounds onto MPs are still unclear. Besides, there is a paucity of multi-dimensional models for predicting the adsorption of organic compounds by MPs under different environmental conditions with a single click. We hope that our review can provide insights into the environmental behavior and fate of organic compounds and microplastics, as well as also guiding future research on the adsorption of organic compounds onto microplastics.