The aggregation-induced emission (AIE) effect is an important feature for luminescence studies, which can offer a broader range of applications for fluorescent materials. Herein, we report the morphological control and photoproperties of amphipathic propeller-shaped rod–coil molecules based on a benzene-1,3,5-tricarboxamide (BTA) unit, which restricts the intramolecular rotation and leads to the AIE effect during the self-assembly process. Investigations on the assembly of these molecules have revealed that tetragonal perforated lamella, hexagonal columnar, body-centered tetragonal micellar, and hexagonal close-packed nanostructures were spontaneously formed in the solid-state. In the solution-state, these molecules assemble into nanosheet-like aggregates, bowl-like objects, and spherical nanoparticles, respectively. The morphology of the molecular aggregates can be controlled by modifying the molecular chain length or introducing lateral methyl groups in the coil chain. Notably, these molecular assemblies exhibit strong AIE phenomena in a mixed THF/H₂O solution and can be used as smart soft materials due to the restriction of their intramolecular motion.