As a floating plant, Myriophyllum aquaticum provides a large surface area under water, and thus has high potential for the removal of pollutants through adsorption. The aim of this study was to evaluate the potential adsorption of tetracycline (TC) by M. aquaticum, and examine the underlying mechanisms. M. aquaticum exhibited a high potential for TC removal from water. Adsorption was the main mechanism for rapid TC removal by live M. aquaticum plants, due to its large contact area and ion exchange, accounting for about 99% and 54% of the total amount of TC removed within 2 h and 5 d, respectively. Further, the roots of M. aquaticum exhibited a higher adsorption capacity than the stems or leaves, as the roots had the largest specific surface area. Fourier transform infrared spectroscopy analysis and identification of functional groups showed that -OH, -COOH, and -NH groups are involved in the adsorption process. The use of M. aquaticum may be a promising approach for TC removal from aquatic environments, especially in terms of shortening reaction times.