HighlightsNiCo/C aerogel was prepared by pyrolysis carbonization self-assembly of NiCo- metal–organic frameworks (MOFs).The assembly mechanism of MOF aerogel was studied by adjusting the ratio of metal ion /BTC.Aerogel combines hydrophobic, lightweight, self-cleaning, and electromagnetic wave absorption properties.Supplementary InformationThe online version contains supplementary material available at 10.1007/s40820-023-01108-3.