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In summary, our results provide a clearer picture of how metal ions co-ordinate, control and thus contribute towards silk protein self-assembly which in turn can inspire structuring approaches in other biopolymer systems.Peptide modified nanoparticles have emerged as powerful tools for enhanced cancer diagnosis and novel treatment strategies. Here, human programmed death-ligand 1 (PD-L1) peptides were used for the first time for the modification of gold nanoprisms (GNPs) to enhance targeting efficiency. A multifunctional nanoprobe was dev