Ac ooperative OSDAs trategy is demonstrated, leading to novel high-silica FAUzeolites with alarge potential for disruptive acid catalysis.I nb ottom-up synthesis,t he symbiosis of choline ion (Ch + )a nd 15-crown-5( CE) was evidenced, in af orm of full occupation of the sodalite (sod) cages with the trans Ch + conformer,i nduced by the CE presence.C Ei tself occupied the supercages along with additional gaucheC h + ,b ut in synthesis without CE, no trans was found. The cooperation, and thus the fraction of trans Ch + ,was closely related to the Si/Al ratio,akey measure for FAU stability and acidity.Assuch, abottom-up handle for lowering the Al-content of FAUa nd tuning its acid site distribution is shown.Amechanistic study demonstrated that forming sod cages with trans Ch + is key to the nucleation of high-silica FAU zeolites.T he materials showed superior performances to commercial FAUz eolites and those synthesized without cooperation, in the catalytic degradation of polyethylene.