The research describes computer-designed uneven peptide particles for pH-responsive assembly into liquid crystals or lattices.[1] These particles use tetrameric helix bundles as basic building blocks, where 11 internal hydrophobic residues provide stability.[1] The assembly is robust over a wide range of pH and temperature and resistant to chemical modifications at the ends of the peptides.[1] At pH 7 in phosphate buffer, peptide P6222 (0.5 mM) forms different structures when cooled to 50 °C or 25 °C.[1] Peptide P2229 (1.0 mM) at room temperature shows different superstructures at pH 7 versus pH 10 in boron buffer.[1] Acetylation of the N-termini allows assembly at low pH, such as pH 4.5 for P2229Ac, or at pH 8 and 50 °C for P4221Ac from 0.1 mM solutions.[1] Control of pH, temperature, primary sequence, and chemical modifications governs the assembly phase and the final morphology of the material.[1]