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Smart molecular probes capable of sensitive,dynamic and multiparameter sensing of molecular changes in complicated biosystems are promising for cancer diagnosis and therapy.To this end,functional evolution of cancer-specific peptides was carried out by the combination of antisense peptide approach and affinity chromatographic screening.An optimal peptide AP2H was identified with high affinity and specificity towards a novel cancer biomarker LAPTM4B protein.By incorporating an aggregation-induced-emission(AIE)fluorophore,a fluorescence turn-on bioprobe(AP2H-TPE)was successfully constructed.The fluorescence signal of AP2H-TPE can be proportionally switched on by the target protein and responsive to the environmental pH as well.Capable of discriminating the expression level of LATM4B protein,AP2H-TPE allows highly specific bioimaging of cancer cells.Real-time monitoring and subcellular localization of LAPTM4B in cancer cells were facilely acquired with a very high target-to-background ratio.Taking advantage of the targetable recognition of AP2H,a dual-functional red-emissive peptide probe TPEred-2AP2H was further developed for the simultaneous fluorescence turn-on bioimaging and photodynamic therapy of tumor cells.Such highly selective peptide probe for molecular signatures of cancer cells can be potential in cancer diagnosis and targetable drug delivery.