New poly(dimethylsiloxane)-based polymer organogelators with L-lysine derivatives were synthesized on the basis of synthetically simple procedure, and their organogelation abilities were investigated. These polymer organogelators have a good organogelation ability and form organogels in many organic solvents. In the organogels, polymer gelators constructed a mesoporous structure with a pore size of about 1 pro formed by entanglement of the self-assembled nanofibers. The L-lysine derivatives in the polymer gelators functioned as a gelation-causing segment and the organogelation was induced by self-assembly of the L-lysine segments through a hydrogen bonding interaction. (c) 2006 Wiley Periodicals, Inc.