The purpose of this study was to investigate the effect of Cu(II) on the adsorption performance and mechanism of tetracycline (TC) adsorption by natural zeolite (NZ) in aqueous solution. Low levels of Cu(II) (<0.01 mmol/L) enhanced the extent of TC adsorption from ∼0.4 mg/g (in the absence of Cu(II)) to ∼0.5 mg/g (with 0.01 mmol/L Cu(II)), resulting in 99% removal of the total TC content. The TC adsorption gradually decreased with increase in the initial pH, but the coexistence of Cu(II) lowered the extent of decrease. The adsorption process was better simulated by the pseudo-second-order kinetics model, but the isotherm model that was more fitting changed from the Langmuir to the Freundlich model as Cu(II) increased, indicating the coexistence of Cu(II) and TC altered the adsorption mechanisms. However, the residual TC in solution increased from 0 to ∼6 mg/L as the concentration of Cu(II) increased from 0 to 1 mmol/L, suggesting a competition between TC and Cu(II) for the adsorption sites in NZ. Fourier transform infrared spectroscopy analysis showed that the functional groups on the surface of NZ changed after the adsorption of TC, suggesting that complex reactions had occurred on the surface of the adsorbent.