An efficient asymmetric Michael reaction of 1,3-dicarbonyl compounds with α-Substituted-β-Nitroacrylates has been developed by using a cinchona-thiourea bifunctional organocatalyst in high yields and enantioselectivies. One of adducts could be transformed into a chiral β-nitroester bearing an isoxazole skeleton and an all-carbon quaternary chiral center.