Given the advantages of being abundant in resources, envi?ronmental benign and highly safe, rechargeable zinc-ion batteries (ZIBs) enter the global spotlight for their potential utilization in large-scale energy storage. Despite their preliminary success, zinc-ion storage that is able to deliver capacity?>?400 mAh g?1 remains a great challenge. Here, we demonstrate the viability of -NH4V4O10 (NVO) as high-capacity cathode that breaks through the bottleneck of ZIBs in limited capacity. The first-principles calculations reveal that layered NVO is a good host to provide fast -Zn2+ ions diffusion channel along its [010] direction in the interlayer space. On the other hand, to further enhance -Zn2+ ion intercalation kinet?ics and long-term cycling stability, a three-dimensional (3D) flower-like architecture that is self-assembled by NVO nanobelts (3D-NVO) is ration?ally designed and fabricated through a microwave-assisted hydrothermal method. As a result, such 3D-NVO cathode possesses high capacity (485 mAh g?1) and superior long-term cycling performance (3000 times) at 10 A g?1 (~?50 s to full discharge/charge). Additionally, based on the excellent 3D-NVO cathode, a quasi-solid-state ZIB with capacity of 378 mAh g?1 is developed.