Here, through the synergism between kinetic dynamic imine-exchange control and thermodynamic control, rarely observed compressible, porous, crystalline covalent organic framework (COF) aerogels were synthesized, the mechanism behind which is a framework crystallization induced self-assembly (FCISA) process. The prepared COF aerogel possessed extremely high BET surface over 2000 m2·g-1 and high maximum equilibrium adsorption capacity toward bisphenol-A of 699 mg·g-1 in aqueous solution.