The invention discloses a high interface adhesion strength nanofiber composite filament bundle and a preparation method and application thereof. The preparation method comprises the following steps: 1, preparing a spinning solution with polymer, additives and solvent, wherein the polymer comprises one or more ingredients out of cellulose diacetate, cellulose triacetate, hydroxyethyl cellulose, polyving akohol and polyving akohol, and the additives comprise one or more ingredients out of ethanediol, glycerol, pentaerythritol, diacetin, glycerol triacetate, glycerol trioleate, glycerol palmitate and glyceryl stearate; 2, taking a cigarette-used filament bundle as base materials, conducting electrostatic spinning on the spinning solution which is obtained in step 1, and obtaining the high interface adhesion strength nanofiber composite filament bundle. By means of the high interface adhesion strength nanofiber composite filament bundle, the phenol release amount and NNK release amount in mainstream smoke of a cigarette can be effectively reduced, the phenol release amount is reduced by 16-30%, and the NNK release amount is reduced by 12-36%.