Since the resumption of highway tolls on May 6, 2020, the national highway network toll collection system based on ETC has been basically stable. With the rapid rise of ETC users, ETC-inefficient transaction increase, which brings great challenges to highway operation services. On the basis of full investigation, this paper analyzes the methods and cases of applying vehicle road cooperation to improve the efficiency of highway toll operation service, puts forward the key work direction to improve the highway operation service level in the future, and discusses the implementation idea of constructing vehicle cooperation service system based on ETC system.