With the advantages of less invasiveness and better shape adaptability, in situ-forming hydrogels are desired biomaterials as scaffolds, drug carriers, and so on. Herein, a negatively charged NaCl-responsive ultrashort peptide sequence (EEH) is reported whose electrostatic repulsion can be reduced through the charge-shielding effect. Under physiological conditions, its AIEgen-capped amphiphile TPE-GEEH of low concentration (1 mg/mL) presents NaCl-triggered morphological transformation from micelle to closely packed fiber with enhanced emission, which can be applied to biosense sodium ion (Na+) with high sensitivity and quick response. At a slightly acidic pH, 10 mg/mL TPE-GEEH undergoes sol-gel transition upon addition of NaCl (100 mM) with improved mechanical properties, which should be useful to develop an in situ-forming hydrogel. Overall, our report provides a simple strategy to construct NaCl-responsive assemblies for potential application in biosensors and drug delivery system.