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Colloidal nanoparticles in tea infusion are the link connecting micromolecular mechanism and macro‐aggregation process of tea cream formation. In order to elucidate, the kinetics mechanism of green tea nanoparticles (gTNPs) aggregation, zeta‐potentials, total average aggregation (TAA) rates, and critical coagulation concentration (CCC) in the presence of various pH and metal ions were investigated. Additionally, the effect of temperature on gTNPs aggregation was further explored. The results revealed that the TAA rate of gTNPs increased with decreasing pH values, the CCC of gTNPs increased in the order Mg2+ ≈ Ca2+ < Na+ ≈ K+. The reason was that different positive ions changed the surface electric field strength of gTNPs to a different extent. Furthermore, it was indicated that low temperature could promote gTNPs aggregation in indirect way. Low temperature promoted the binding of epigallocatechin gallate (EGCG) and caffeine, and the combination between gTNPs and EGCG–caffeine complexes weakened the stability of gTNPs resulting from reduction in electrostatic repulsion. Practical Application: Tea is a popular beverage all over the world. This research revealed the mechanism of green tea nanoparticles aggregation and laid a theoretical foundation for the regulation of tea cream formation in tea beverage. [ABSTRACT FROM AUTHOR]