To trigger a thermo-reversible gelation, we found that covalent functionalization of PEDOT:PSS with PNIPAM was necessary, as a control experiment showed that blending PEDOT:PSS with PNIPAM, as has been done in solid films, resulted in only the precipitation of PNIPAM without gelation of PEDOT:PSS. We also found that the block copolymer structure is essential for the solgel transition. A random copolymer of PSS with PNIPAM (Scheme S4) used to prepare PEDOT:PSS-co-PNIPAM (Scheme S5), with identical mass ratios of all components as in the TR-CP, only displayed a slight increase in viscosity on heating. These control experiments highlight the need for a controlled block copolymer architecture to achieve the desired reversible gelation.