Water soluble polyacylhydrazones have been generated that contain a high proportion of renewable materials. The polyacylhydrazones were found to be present simultaneously as linear and macrocyclic species, the latter being favoured at higher concentrations and in certain combinations of levulinoyl ester/acyldihydrazide. Levulinoyl esters with multiple ketone reactive sites were targeted as building blocks for the backbone. Reaction of these species in aqueous media with commercially available acyldihydrazides afforded a series of high solids-content water soluble polyacylhydrazone solutions. Evaporation of the water from the solutions reproducibly generated films with differing and useful characteristics. One of the polyhydrazones was successfully formulated into two different types of resin bases of commercial coating systems, producing paint products with renewable content. Supporting Information. Proton, carbon and 2D-NMR spectra for key di-and tri-levulinoyl esters and mono-and diacylhydrazones. This material is available free of charge via the Internet at http://pubs.acs.org.