The present invention relates to a cellulose nano-fibril/epoxy resin composite film preparation method, which comprises the following steps: a) purifying a raw material; 2) carrying out chemical treatments, wherein the chemical treatments comprise three acid treatments and two alkali treatments; 3) carrying out physical treatments, wherein the physical treatments contain three mechanical treatments such as ultrasonic crushing, grinding through a grinding machine, and a high pressure homogenizer; 4) preparing a fiber nano-fibril film; and 5) preparing a cellulose nano-fibril/epoxy resin composite material. According to the present invention, the prepared cellulose nano-fibril has a diameter of 20-80 nm, the nano-cellulose film has a tensile strength of 159.2 MPa and an elastic modulus of 7.3 GPa, transmittance of the nano-cellulose resin film is 86%, the cellulose film has characteristics of high length-diameter ratio, uniform fiber diameter distribution, good thermal stability, and a thermal expansion coefficient of 14 ppm/K, and the film can be widely applied in the fields of high temperature resistance flexible electronic device light transmittance films, optically transparent functional paper, gas barrier packaging materials, tissue engineering materials, filtration membrane materials and the like.