Polydopamine (PDA) is a synthetic polymeric material with immense potential in biomedical and surface functionalization applications. Herein, we have screened self‐assemblies formed by Phenylalanine‐based amphiphiles (Phe‐AMPs) as soft templates for preparing chiral PDA nanostructures. Our study revealed that the amphiphile 2 endowed with a primary amine residue afforded chirally‐twisted ultrathin nanoribbons of PDA under optimized conditions. The chirality at the Phe residue of 2 modulated the twist‐chirality of the PDA nanoribbons; the l‐2 resulted in nanoribbons with right‐handed twist, whereas the d‐2 induced a left‐handed twist to the ribbons. The racemic mixture of these two amphiphiles produced flat, achiral tapes. The PDA ribbon thickness was ≈5.86±0.40 nm, whereas its width and length were ≈133.5±3.2 nm and >5000 nm, respectively. Upon dialysis, hollow PDA nanotubes were obtained due to curling of the PDA nanoribbons. These PDA‐nanoarchitectures were employed to spontaneously form and assemble Ag‐nanoparticles along the edges of the PDA nanoribbons. In this work we are reporting chirality controlled synthesis of PDA nanostructures for the first time.