The invention provides a multi-responsive intelligent nano fiber functional material and a preparation method and application thereof. The method utilizes two temperature sensitive monomers of N-isopropyl acrylamide and N-vinyl caprolactam to simultaneously modify polyethyleneimine, and re-grafts the polyethyleneimine onto cellulose nanofibers to prepare the multi-responsive intelligent nanofiberfunctional material with good pH responsiveness and temperature responsiveness. The material can achieve the intelligent transformation of super-hydrophilic and super-hydrophobic and super-lipophilicand super-oleophobic under a temperature and pH stimulus responsiveness condition, and the low critical solution temperature of the material can be controllably adjusted in the range of 30.5-31.5 DEGC. The multi-responsive intelligent nano fiber functional material can be widely applied to the fields of drug sustained release, oil-water separation and the like.