Interfacial solar evaporation holds immense potential for brine desalination with low carbon footprints and high energy utilization. Hydrogels, as a tunable material platform from the molecular level to the macroscopic scale, have been considered the most promising candidate for solar evaporation. However, the simultaneous achievement of high evaporation efficiency and satisfactory tolerance to salt ions in brine remains a challenging scientific bottleneck, restricting the widespread application. Herein, we report ionization engineering, which endows polymer chains of hydrogels with electronegativity for impeding salt ions and activating water molecules, fundamentally overcoming the hydrogel salt-impeded challenge and dramatically expediting water evaporating in brine. The sodium dodecyl benzene sulfonate-modified carbon black is chosen as the solar absorbers. The hydrogel reaches a ground-breaking evaporation rate of 2.9 kg m-2 h-1 in 20 wt% brine with 95.6% efficiency under one sun irradiation, surpassing most of the reported literature. More notably, such a hydrogel-based evaporator enables extracting clean water from oversaturated salt solutions and maintains durability under different high-strength deformation or a 15-day continuous operation. Meantime, on the basis of the cation selectivity induced by the electronegativity, we first propose an all-day system that evaporates during the day and generates salinity-gradient electricity using waste-evaporated brine at night, anticipating pioneer a new opportunity for all-day resource-generating systems in fields of freshwater and electricity.