A novel type of stimuli-responsive dynamic helical polymer–metal nanoparticle nanocomposite formed by a helical poly(phenylacetylene) (PPA) combined with gold nanoparticles (AuNPs) is described. Thus, several PPA copolymers containing the ethynyl-4-benzamide of (S)-phenylglycine methyl ester (M1) to dictate the helical structure/sense of the copolymer, and the ethynyl-4-benzamide of the 11-((2-(2-(2-aminoethoxy)ethoxy)ethyl)amino)undecane-1-thiol (M2) to link the copolymer to the AuNPs are prepared. Different morphologies of these nanocomposites were obtained by considering the thiol ratio and the self-assembly properties of the PPA, which generates from dispersed AuNPs to fibre-like structures. All these nanocomposites show a dynamic chiral behaviour, it being possible to manipulate their helical sense by the action of external stimuli. Moreover, it is possible to control the aggregation of these nanocomposites into macroscopically chiral nanospheres with low polydispersity by using Ba2+ as a crosslinking agentWe thank Servicio de Microscopía Electrónica (RIAIDT, USC). Financial support from MINECO (CTQ2015-70519-P), Xunta de Galicia (ED431C 2018/30, Centro singular de investigación de Galicia accreditation 2016-2019, ED431G/09) and the European Regional Development Fund (ERDF) is gratefully acknowledged. M. N.-M. thanks MICINN for an FPI contract (BES-2016-078107)S
