Self-Assembly for Ultrasensitive Detection In article number 2314832, Hai Zhang, Xiaofei Chen, Quan Li, and co-workers report a peptide-derived supramolecular self-assembly system for ultrasensitive and visual detection of heparin in vivo. Two peptides are designed and modified by gold nanocluster and tetraphenylethene to co-assemble into nanoparticles for co-recognition of heparin. The new approach reaches an extreme low limit of detection and dramatic fluorescence color change to be simply distinguished on paper by naked eye.