Modifying the surfaces of zinc and other metallic substrates is considered an effective strategy to enhance the reversibility of the zinc deposition and stripping processes. While a variety of surface modification strategies have been explored, their ability to be practically implemented is not always trivial due to the associated high costs and complexity of the proposed techniques. In this study, we showcase a straightforward method for preparing ultrathin polyelectrolyte coatings using polydiallyldimethylammonium chloride (PDDA) and polyethylenimine (PEI). The coatings, characterized by their electrostatic charge and hydrophobicity, suppress side reactions and even out the electrodeposition process across the substrate surface. The PDDA-coated anodes demonstrate significantly reduced voltage hysteresis, uniform zinc morphology, improved self-discharge rates, and an impressive Coulombic efficiency exceeding 99% over prolonged cycling. Our findings highlight the potential that such cost-effective and straightforward surface treatments could be widely applied in Zn metalbased batteries.