Insight　is　provided　into　the　mechanism　of　peptide　gelation,　a　self-assembled　process　of　particular　interest,　due　to　its　wide　existence　in　natural　events　and　broad　applications　in　food　and　biomaterials　field,　but　hard　to　control　as　minor　alterations　in　the　peptide　sequence.　Here,　we　design　a　family　of　pentapeptides　and　control　their　selfassembly　behaviors,　from　micro-　and　nanoparticles　to　nanofibers　and　hydrogels.　Furthermore,　based　on　the　thermodynamics,　the　gelation　kinetics　and　the　ionization　status　of　terminal　groups,　the　peptide　assembly　goes　through　five　stages　as　varying　the　pH　value　and　the　assembly　structures　are　highly　dependent　on　the　charging　status　of　the　terminal　groups.　The　gelation　rules　of　these　peptides　are　further　investigated.　Besides,　we　also　load　hydrophobic　functional　molecule　(curcumin)　into　different　self-assembly　nanostructures　with　high　encapsulation　efficiency　and　remarkable　thermal　and　light　protection　on　curcumin.　These　peptides　assemblies　with　tunable　structures,　encapsulation　ability　and　photothermal　stabilization　could　become　promising　candidates　for　hydrophobic　function　factor　delivery　in　food　industry.