The invention provides a method for organically catalyzing asymmetric functionalization of inactive sp3 carbon-hydrogen bonds of indole and applications. A catalyst used in the method comprises an organic acid catalyst and an organic urea catalyst. The organic acid catalyst is diphenyl phosphate, the organic urea catalyst is (2S)-2-[[[[3,5-bis(trifluoromethyl)phenyl]amino]oxomethyl]amino]-N-(diphenylmethyl)-N-3,3-trimethyl butylamide, and the structural formula of the organic urea catalyst is shown in the specification. By adding the organic acid catalyst and the organic urea catalyst, the asymmetric functionalization reaction of the non-activated sp3 carbon-hydrogen bond on indole can be realized at normal temperature and normal pressure.