The invention relates to the field of tunnel engineering construction equipment, and discloses a plug structure mounted between a template trolley and surrounding rock, and a mounting method of the plug structure. The plug structure is characterized in that a first elastic material layer, an inner ring reinforcing steel bar, a second elastic material layer, a buried type water stop band, a third elastic material layer, an outer ring reinforcing steel bar and an inflatable layer are annularly laid in sequence at the end part of the template trolley towards the surrounding rock. By use of the inflating pressure of the inflatable layer and the elastic characteristics of the multiple elastic material layers, interlayer structures of a plug can be tightly squeezed together, so that the reinforcing steel bars and the water stop band can be exposed out of the plug structure, mold-shut construction is facilitated, staggering of the water stop band is prevented; furthermore, no gap exists in the plug structure, so that slurry leakage during model forming is avoided; meanwhile, no damage to a waterproofing plate below the surrounding rock at the top is caused, and the potential hazard of water leakage of a tunnel can be eliminated.