A method for efficiently eliminating graphene wrinkles formed by chemical vapor deposition includes: directly growing super smooth wrinkle-free graphene films on metal substrates such as copper, nickel and alloys thereof and non-metal substrates such as silicon oxide and silicon carbide, or eliminating the wrinkles of wrinkled graphene through controlled proton injection at a high temperature by precisely controlling the temperature and hydrogen plasma power and time for generating protons; where the plasma-assisted chemical vapor deposition system includes a plasma generator, a vacuum system and a heating system; where the power of the plasma generator is 5 to 1000 W, the pressure of the vacuum system is 10−5 to 105 Pa, and the heating temperature of the system is controllable between 25 to 1000° C.; directly growing a super smooth wrinkle-free graphene by injecting protons on various substrates during growth.