The invention discloses a preparation method of a metal nanoparticle modified graphene composite material. The preparation method comprises the steps of preparing a graphene flake and a metal nanoparticle: firstly, mixing the graphene flake, the metal nanoparticle and ethanol according to the mass ratio of (1-3): (50-100): (500-1000), and carrying out ultrasonic treatment for at least 10min to obtain a mixed solution; then, centrifuging the mixed solution at the rotating speed of 12000-16500r/min for at least three times to obtain the metal nanoparticle modified graphene composite material, wherein the lasting time for centrifuging every time is at least 10min, the metal nanoparticle is modified on the graphene flake, the graphene flake has the length of 2-4mu m, the width of 1-3mu m and the thickness of less than or equal to 1nm, the metal is one of silver, gold, palladium, platinum, copper, ferrum, cobalt and nickel, and the nanoparticle is one of a nanosphere, a triangular nanoplate, a nanocube and a nanorod. The preparation method is not only convenient and rapid, but also capable of ensuring that the metal nanoparticle in the prepared metal nanoparticle modified graphene composite material is controllable in appearance.