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The dephasing time of localized surface plasmons is a crucial parameter that defines the quality of resonance and achievable electromagnetic field enhancement near metal nanoparticles. Lattice irregularities of as‐deposited supported metal nanoparticles shorten the plasmon dephasing time and degrade the resonance quality. To study the crystallinity influence on the plasmon dephasing time in more detail, silver nanoparticles in the form of a granular film were produced on dielectric substrates via physical vapor deposition in a vacuum chamber. The samples are characterized using Vis–NIR spectroscopy and transmission electron microscopy. The persistent spectral hole burning technique is applied to study the annealing influence on the dephasing time of localized surface plasmons of the particular resonance frequency. After annealing, the improved crystallinity of nanoparticles leads to a twofold dephasing time increase. This conclusion is supported by the electron diffraction patterns. The role of the improved crystallinity among concurrent effects of annealing is discussed.

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