Aqueous zinc-ion batteries (ZIBs) have shown great potential in the fields of wearable devices, consumer electronics, and electric vehicles due to their high level of safety, low cost, and multiple electron transfer. The layered cathode materials of ZIBs hold a stable structure during charge and discharge reactions owing to the ultrafast and straightforward (de) intercalation-type storage mechanism of Zn²⁺ ions in their tunable interlayer spacing and their abilities to accommodate other guest ions or molecules. Nevertheless, the challenges of inadequate energy density, dissolution of active materials, uncontrollable byproducts, increased internal pressure, and a large de-solvation penalty have been deemed an obstacle to the development of ZIBs. In this review, recent strategies on the structure regulation of layered materials for aqueous zinc-ion energy storage devices are systematically summarized. Finally, critical science challenges and future outlooks are proposed to guide and promote the development of advanced cathode materials for ZIBs.