The development of new porous materials has attracted intense attention as adsorbents for removing pollutants from wastewater. However, pure inorganic and organic porous materials confront various problems in purifying the wastewater. In this work, we integrated a covalent organic framework (TpPa-1) with an inorganic zeolite (TS-1) for the first time via a solvothermal method to fabricate new-type nanoadsorbents. The covalent organic framework/zeolite (TpPa-1/TS-1) nanoadsorbents combined the merits of the zeolite and COF components and possessed efficient adsorptive removal of organic contaminants from solution. Structural morphology and chemical composition characterization by powder X-ray diffraction, scanning electron microscopy, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, transmission electron microscopy and thermogravimetric analysis demonstrated the successful preparation of TpPa-1/TS-1 composite nanoadsorbents. The resultant composite adsorbent TpPa-1/TS-1 removed rhodamine B at 1.7 and 2.6 times the efficiency of TpPa-1 and TS-1, respectively. Additional investigation revealed that the Freundlich adsorption isotherm and the pseudo-second-order kinetic model could be employed to represent the adsorption process more appropriately. Thermodynamic calculation analysis showed that the adsorption process proceeded spontaneously and exothermically. Besides, the effects of pH, absorbent mass and ionic strength on the adsorption performance were systematically investigated. The prepared composite adsorbent showed a slight decrease in removal efficiency after eight cycles of repeated use, and real water environment experiments also showed the high stability of the adsorbent. The enhanced performance can be attributed to electrostatic interaction, acid-base interaction, hydrogen bonding and π-π interactions.