The preparation of nanoparticles consisting of chiral helical substituted polyacetylenes via emulsification of the preformed polymers is reported. Two types of helically substituted acetylenes were examined as model polymers: two chiral poly(N‐propargylamide)s and two achiral poly(N‐propargylamide)s. The four polymers were emulsified with SDS as emulsifier to form nanoparticles. The particle size can be modulated by varying the SDS concentration. A comparison between nanoparticle emulsion and the corresponding polymer solution demonstrated obvious blue shifts in the CD spectra of nanoparticle emulsions made from helical polymers with relatively not‐so‐bulky pendent groups, for which the possible mechanism was proposed.