Graphical Abstract Phase-Separated Polyzwitterionic Hydrogels In article number 2214045, Lianbin Zhang and co-workers construct a polyzwitterionic hydrogel evaporator with tunable sponge-like structures by a phase separation strategy for stable solar steam generation. Owing to the anti-polyelectrolyte effects and the highly interconnected pore structure, the evaporator enables adequate seawater uptake and transport to ensure a fast and stable water evaporation process.