Azomethine ylides are useful intermediates for the rapid construction of chiral N-containing com-pounds.However,its synthetic potential has not been fully developed due to the limited reaction models.In combination with synergistic catalysis and azomethine ylide chemistry,we have devel-oped several types of novel catalytic system in-cluding Cu/Pd,Cu/Ir and PTC/Ir catalysis,which can convert readily-available azomethine ylides to various high-valued molecules such as unnaturalα-amino acids,homoallylic amines and N-heterocycles.Compared with the traditional mono-catalysis,the synergistic catalyst system exhibits en-hanced catalytic efficiency and chiral induction ability in many cases.In addition,we have demonstrated that these strategies could be applied in the construction of bioactive compounds and natural products.