Polycyclic aromatic hydrocarbon (PAH) molecules may play an essential role in the prebiotic compound evolution network in interstellar clouds. In this work, an experimental study of large, astronomically relevant PAH-organic molecule clusters is presented. With the initial molecular precursors dicoronylene (DC; C 48 H 20 )-pyroglutamic acid (Pga, C 5 H 7 NO 3 ), DC-proline (Pro; C 5 H 9 NO 2 ), and DC-pyroglutaminol (Pgn; C 5 H 9 NO 2 ), our experiments indicate that PAH-organic molecule cluster cations (e.g., (Pga) (1−2) C 48 H n + , (Pro) (1−2) C 48 H n + , and (Pgn) (1−6) C 48 H n + ) and carbon cluster-organic molecule cluster cations (e.g., (Pga)C 48 + , (Pro) (1−2) C 48 + , and (Pgn) (1−6) C 48 +) are gradually formed through an ion-molecule collision reaction pathway in the presence of a strong galactic interstellar radiation field. These laboratory studies provide a gas-phase growth route toward the formation of complex prebiotic compounds in a bottom-up growth process, as well as insight into their chemical-evolution behavior in the interstellar medium.