We report the helix‐sense‐selective memory polymerization (HSMP) of achiral biphenylylacetylenes bearing carboxy and amino pendant groups in the presence of basic and acidic chiral guests in water, respectively. The HSMP proceeds in a highly helix‐sense‐selective manner driven by noncovalent chiral ionic interactions between the monomers and guests under kinetic control, producing the one‐handed helical polymers with a static memory of helicity in one‐pot during the polymerization in a very short time, accompanied by amplification of asymmetry. The carboxy‐bound helicity‐memorized polymer self‐assembles into a cholesteric liquid crystal in concentrated water, in which a variety of basic achiral fluorophores further co‐assembles to form supramolecular helical aggregates that exhibit an induced circularly polarized luminescence in a color tunable manner.