Ultrafine gaps in metal nanostructures are highly important in nano optoelectronic devices. The synergistic deformation process of metal nanostructures and aluminium films under laser shock through molecular dynamics simulations and experiments was investigated, revealing the formation and adjustment mechanism of ultrafine wire gaps. The simulation results show that the high strain rate deformation generated by laser shock causes the radial expansion of metal nanoparticles, whereas the aluminium film flows towards the nanoscale gaps under the action of shock waves, forming nanoscale protrusions that prevent the fusion of nanoparticles. The squeezing effect between the aluminium film and the gold nanoparticles provides an additional restraining force, making the deformation of the metal nanostructure more uniform and forming stable ultrafine wire gaps. By adjusting the laser energy and nanostructure parameters, the gap size can be precisely controlled, providing a theoretical basis for the high-precision preparation of ultrafine gaps in metal nanostructures.