We introduce poly(1,6-pyrene terephthalamide) polymer (PPyrTA) as an aromatic polyamide analogue of poly(p-phenylene terephthalamide) (PPTA), also known as Kevlar®. This work shows that the incorporation of polycyclic aromatic pyrene moieties improves drastically the mechanical properties of the polymeric structure, increasing elastic nanoindentation-determined modulus and hardness by factors of 1.9 and 4.3, respectively. Liquid deprotonated dispersions of PPyrTA nanofibers were used as nanoscale building block for producing large-surface, free-standing polymer macroscopic nanofilms. This 2D assembly leads to further significant improvements in reduced modulus and hardness (more than twice) compared to the starting polymer macroscale fibres, due to a better re-organizational arrangement of the PPyrTA nanofibers in the nanofilms, formed under 2D spatial confinement.
