Anisotropic polymer-inorganic composite latex particles were synthesized by using a RAFT-based encapsulation approach on cationic gibbsite platelets. By using the RAFT agent dibenzyl trithiocarbonate, a series of amphipatic living random RAFT copolymers with different combinations of acrylic acid and butyl acrylate units were synthesized. These RAFT copolymers were used as living stabilizers for the gibbsite platelets and chain extended to form a polymeric shell by starved feed emulsion polymerization. Cryo-TEM characterization of the resulting composite latexes demonstrates the formation of anisotropic composite latex particles with mostly one platelet per particle. Monomer feed composition, chain length, and hydrophilic-lipophilic balance...