This review summarizes recent advances in the design and synthesis of amino-acid-based block copolymers by reversible addition-fragmentation chain transfer (RAFT) polymerization of amino-acid-bearing monomers. We will mainly focus on stimuli-responsive block copolymers, such as pH-, thermo-, and dual-stimuli-responsive block copolymers, and self-assembled block copolymers, including amphiphilic and double-hydrophilic block copolymers having tunable chiroptical properties. We will also highlight recent results in RAFT synthesis of amino-acid-based copolymers having various properties, such as catalytic and optoelectronic properties, cross-linked block copolymer micelles, unimolecular micelles, and organic-inorganic hybrids.