This work investigated the polyanion-initiated gelation process in fabricating chitosan-tripolyphosphate (CS-TPP) nanoparticles intended to be used as carriers for delivering tea catechins. The results demonstrated that the particle size and surface charge of CS-TPP nanoparticles could be controlled by fabrication conditions. For preparation of CS-TPP nanoparticles loaded with tea catechins, the effects of modulating conditions including contact time between CS and tea catechins, CS molecular mass, CS concentration, CS-TPP mass ratio, initial pH value of CS solution, and concentration of tea catechins on encapsulation efficiency and the release profile of tea catechins in vitro were examined systematically. The study found that the encapsulation efficiency of tea catechins in CS-TPP nanoparticles ranged from 24 to 53%. In addition, FT-IR analysis showed that the covalent bonding and hydrogen bonding between tea catechins and CS occurred during the formation of CS-TPP nanoparticles loaded with tea catechins. Furthermore, studies on the release profile of tea catechins in vitro demonstrated that the controlled release of tea catechins using CS-TPP nanoparticles was achievable.