Two poly(benzyl ether) dendrons,decorated in their periphery with nitrile groups,were divergently synthesized and fully characterized.Their gelation properties were studied by using scanning electron microscopy(SEM),X-ray crystal structure analysis and concentration-and temperature-dependent 1 H NMR spectroscopy.It was found that the gelation capability of these dendrons was highly dependent on dendron generation,and the second-generation dendron G 2-CN proved to be highly efficient organogelator despite the lacking of any conventional gelation motifs,such as amides,long alkyl side chains and steroidal groups.The multiple strong-stacking interactions and hydrogen bonding interactions due to the peripheral isophthalonitrile motifs were proved to be the main driving forces to form the self-assembled gel.