Chiral self-sorting is intricately connected to the complicated chiral processes observed in nature and no artificial systems of comparably complexity have been generated by chemists.H owever,o nly af ew examples of purely organic molecules have been reported so far,w here the selfsorting process could be controlled. Herein, we describe the chiral self-sorting of large cubic [8+ +12] salicylimine cage compounds based on ac hiral TBTQ precursor.O ut of 23 possible cage isomers only the enantiopure and am eso cage were observed to be formed, whichhave been unambiguously characterized by single crystal X-raydiffraction. Furthermore, by careful choice of solvent the formation of meso cage could be controlled. With internal diameters of d in = 3.3-3.5 nm these cages are among the largest organic cage compounds characterizedand show very high specific surface areas up to approx. 1500 m 2 g À1 after desolvation.