Description:
<jats:title>Abstract</jats:title><jats:p>The synthesis of ABA and ABA′ triblock polyethylene glycol‐and polysarcosine‐peptide conjugates is reported. The A/A′ peptides are based on phenylalanine(F)‐histidine(H) pentapeptide sequences FHFHF, which promote pH‐switchable β‐sheet self‐assembly into nanorods in water. Only parallel β‐sheet‐driven folding and intermolecular assembly using ABA triblock polymer–peptide conjugates leads to interstrand cross‐linking and hydrogelation, highlighting the impact of supramolecular interactions‐directed structure formation at the nano‐ and mesoscopic level.</jats:p>