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Biomimetic design to afford smart functional biomaterials with exquisite properties represents synthetic challenges and provides unique perspectives. In this context, elastin‐like polypeptides (ELPs) recently became highly attractive building blocks in the development of lipoprotein‐based membranes. In addition to the bioengineered post‐translational modifications of genetically encoded recombinant ELPs developed so far, we report here a simple and versatile method to design biohybrid brush‐like lipid‐grafted‐ELPs using chemical post‐modification reactions. We have explored a combination of methionine alkylation and click chemistry to create a new class of hybrid lipoprotein mimics. Our design allowed the formation of biomimetic vesicles with controlled permeability, correlated to the temperature‐responsiveness of ELPs. [ABSTRACT FROM AUTHOR]