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Fast optical modulation of nanoplasmonics is fundamental for on-chip integration of all-optical devices. Although various strategies have been proposed for dynamic modulation of surface plasmons, critical issues of device compatibility and extremely low efficiency in the visible spectrum hamper the application of optoplasmonic nanochips. Here we establish an optoplasmonic system based on Au@Cu2–xS hybrid core–shell nanoparticles. The optical excitation of hot electrons and their charge transfer to the semiconductor coating (Cu2–xS) lead to lowered electron density of Au, which results in the red shift of the localized surface plasmon resonance. The hot electrons can also transport through the Cu2–xS layer to the metal substrate, which increases the conductance of the nanogap. As such, the coupled gap plasmon blue-shifts with a magnitude of up to ∼15 nm, depending on the excitation power and the thickness of the coatings, which agrees with numerical simulations. All of this optoelectronic tuning process is highly reversible, controllable and fast with a modulated laser beam, which is highly compatible and sufficiently useful for on-chip integration of nanophotonic devices. [ABSTRACT FROM AUTHOR]