Upon stimuli-triggered single cleavage of capping moieties at the focal point and chain terminal, self-immolative dendrimers (SIDs) and linear self-immolative polymers (/-SIPs)undergo spontaneous domino-like radial fragmentation and cascade head-to-tail depoly-merization, respectively.The nature of response selectivity and signal amplification has rendered them an unique type of stimuli-responsive materials.Moreover, novel design principles are required for further advancement in the field of self-immolative polymers (SIPs).