(A) Molecular structures of NapFFpYGGaa (1P, Nap: naphthylacetic acid; F: L-phenylalanine; pY: L-phosphotyrosine; G: glycine; a: D-alanine), vancomycin (2), and their non-covalent complex 1P:2. (B) Illustration of the context-dependent dynamic continuum of molecular assemblies for controlling cell fate. By controlling the activity of the ectophosphatase (e.g., ALPL) on cancer cells via a corresponding enzyme inhibitor, dynamic continuum of the assemblies of supramolecular phosphoglycopeptides (sPGP) resulting in a 2D cell sheet, 3D cell spheroids, or cell death.