The　treatment　of　surfactant-stabilized　oily　wastewater　and　organic　dyes　remains　a　global　sustainability　challenge　due　to　the　high　energy　consumption　and　secondary　pollution　of　conventional　methods　(e.g.,　chemical　demulsification　and　membrane　filtration.　Biomass-derived　cellulose　aerogels　offer　promise　due　to　their　renewability　and　adjustable　wettability;　however,　their　practical　application　is　hindered　by　intrinsic　brittleness,　structural　collapse　during　ambient　drying,　and　insufficient　mechanistic　understanding.　Herein,　we　report　a　structurally　reinforced,　multifunctional　cellulose–metal　composite　aerogel　(APCAM),　fabricated　via　a　scalable　tri-phase　strategy　that　integrates　Schiff-base　crosslinking,　silane-induced　nanoscale　locking,　and　a　programmable　metallic　rubber　scaffold.　This　dual-network　architecture—comprising　a　self-crosslinked　siloxane　matrix　and　an　embedded　elastic　metal　framework—enables　ambient　drying,　multiscale　energy　dissipation,　prestress　compensation,　and　hierarchical　deformation　adaptability.　The　resulting　APCAM　exhibits　superhydrophilicity　and　underwater　superoleophobicity　(0°/154°),　along　with　exceptional　fatigue　resistance,　retaining　89　%　of　its　original　strength　after　10,000　compression　cycles　at　30　%　strain.　Functionally,　it　combines　high-performance　emulsion　demulsification　(＞99.98　%),　rapid　flux　(4398　L·m−2·h−1),　significant　dye　adsorption　capacity　(395　mg/g),　and　thermal　insulation.　Computational　fluid　dynamics　(CFD)　simulations　reveal　that　stratified　porous　networks　and　microscale　vortices　facilitate　droplet　coalescence　and　repulsion　through　energy　barrier　modulation.　The　material　maintains　a　flux　＞3560　L·m−2·h−1　after　50　reuse　cycles,　with　degradation　©　2025　Elsevier　B.V.