Batch experiments were conducted to investigate the effects of tea polyphenols, Cu and pH on the releases of Ca and Mg from two variable-charge soils (an Oxisol and an Ultisol). When the initial concentration of Cu was 2.0 mmol/L and the final system pH was 5.0, the releases of Ca and Mg from variable-charge soils decreased with the dosage increase of tea polyphenols, because of the surface negative charge was increased due to the presence of tea polyphenols. When the initial concentration of tea polyphenols was 20 g/kg and the final system of pH was 5.0, the releases of Ca and Mg from invariable-charge soils increased with the increase of initial concentration of Cu. The increase of initial concentration of Cu increased the adsorption of Cu by variable-charge soils. Cu exchanged with adsorbed Ca and Mg on the soils and competed for adsorption sites with Ca and Mg, which enhanced the releases of Ca and Mg from the two soils. When the initial concentration of tea polyphenols was 20 g/kg and initial concentration of Cu was 2.0 mmol/L, the releases of Ca and Mg from variable-charge soils decreased with the increase of suspension pH due to the increase in negative surface charge on the soils and electrostatic adsorption of Ca and Mg by the soils. At the same pH, tea polyphenols increased the negative charge of variable-charge soils and thus reduced the releases of Ca and Mg from variable-charge soils. The results above can provide useful references for the control of soil acidification and heavy metal pollution in tea gardens.