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We study the plasmonic properties of hybrid nanostructures consisting of double vacancy defected graphene (DVDGr) and metallic nanoarrays using the time-dependent density functional theory. It is found that DVDGr with pure and mixed noble/transition-metal nanoarrays can produce a stronger light absorption due to the coherent resonance of plasmons than graphene nanostructures. Comparing with the mixed Au/Pd nanoarrays, pure Au nanoarrays have stronger plasmonic en-hancement. Furthermore, harmonics from the hybrid nanostructures exposed to the combination of lasers ranged from ultraviolet to infrared and a controlling pulse are investigated theoretically. The harmonic plateau can be broadened signifi-cantly and the energy of harmonic spectra is dramatically extended by the controlling pulse. Thus, it is possible to tune the width and intensity of harmonic spectrum to achieve broadband absorption of radiation. The methodology described here not only improves the understanding of the surface plasmon effect used in a DVDGr-metal optoelectronic device but also may be applicable to different optical technologies.