The invention discloses a nanofiber composite filament bundle with high interfacial adhesion strength and its preparation method and application, wherein the preparation method comprises the following steps: (1) preparing a polymer, an additive and a solvent into a spinning solution; the polymer It is at least one of cellulose diacetate, cellulose triacetate, hydroxyethyl cellulose, polyvinyl alcohol, chitosan; the additive is ethylene glycol, glycerol, pentaerythritol, glyceryl diacetate, three At least one of glyceryl acetate, glycerol trioleate, glyceryl palmitate, glyceryl stearate; (2) taking tobacco tow as the base material, the spinning solution obtained in step (1) is processed Electrospinning to obtain the composite tow of nanofibers with high interfacial adhesion strength. The nanofiber composite tow with high interfacial adhesion strength disclosed by the invention can effectively reduce the release of phenol and NNK in cigarette mainstream smoke, the release of phenol is reduced by 16-30%, and the release of NNK is reduced by 12-36%.