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Motivation: Proteins, and their shorter ‘cousins’ peptides, are the building blocks of life, providing dynamic structures and functions from the molecular to the macro-scale in living systems. Yet, creating stable, designed materials with them remains a challenge.

Achievements: We designed peptide ‘patchy particles’ with patterned surface charge to program ordered, stable materials across a broad pH range (1-14). At low pH, liquid crystals formed with different phases at low concentrations of building block (nematic) versus higher concentrations (hexagonal columnar).

Importance: This work shows how charges are arranged on a peptide particle surface, not just its composition, governs how it assembles for the predictable control of biomolecular assemblies across extreme conditions.

MRSEC relevance: This contribution advances the design of responsive, hierarchical biomaterials through collaborative team science: a versatile platform for making soft materials that function under harsh conditions with protein-like specificity and control and future opportunities for use as nano-actuators to do work.