Photoresponsive molecular assembly based on diarylethene (DAE) is an interesting class of supramolecular system as it can allow remarkable morphological transition via small structural changes upon photoisomerization. Herein, we report coassemblies of diarylethene and perylene bisimide through complementary multiple hydrogen-bonding. The open isomer of the diarylethene and the perylene bisimide coassemble to afford photoresponsive helical supramolecular polymer nanofibers. The ring-closure photoreaction of the diarylethene unit enables transformation of helical nanofibers to non-helical fibers. The non-helical fibers can only be obtained through the photoisomerization, and are never achievable by thermal coaggregation of the close isomer and the perylene bisimide. This study illustrates that the proper incorporation of photochromic units into a non-equilibrated molecular assembly system achieved by strong intermolecular interaction enables us to design new self-assembled products in terms of morphology and functions, which are not obtainable through the self-assembly of ground state molecules under either kinetic or thermodynamic control.