Large-area plasmonic photonic structures containing a proportion of quasicrystals can be fabricated by a solution-processable method. A photoresist film is exposed to a multi-beam interference pattern to form a quasicrystal template. A gold nanoparticle colloid is then spin-coated onto the template. An inverse pattern can be obtained after annealing to afford greater control over the sample morphologies and spectroscopic characteristics. Coupling between the waveguide modes and particle plasmons strengthens with increasing annealing temperature. After mode degeneration is removed, a multi-mode coupling process is observed. These results are helpful in understanding the mechanisms and design strategies of complex plasmonic nanostructures.