Abstract: Addition of macromolecular templates to Polymer-Scaffolded Dynamic Combinatorial Libraries (PS-DCLs) constructed by the reversible conjugation of acylhydrazides onto aldehyde-functionalised polymer scaffolds has been shown to generate a population of polymers with enhanced binding affinities towards templates, as determined by a fluorescence-based method. The templating process, which harnesses electrostatic interactions between library members and templates, has been shown to be reversible, with PS-DCLs returning to their initial composition upon removal of the template. Solid-supported templates have been employed for the convenient isolation of the best-binding fraction of the library