Abstract This paper presents a voltage-induced and thermal annealing rearrangement (VITAR) method based on modified Electric Field Assisted Film Dissolution (EAFD) method as a flexible and powerful tool for manipulating nanoparticles spatial distribution based on drift and diffusion mechanisms that occur due to external DC voltage and thermal annealing processes. Different samples with various arrangements of external DC voltage and thermal annealing processes have been produced. The extinction and attenuated total reflection (ATR) spectra, as well as Atomic Force Microscope (AFM) images, have been employed to investigate their optical and morphological properties. Four cases with arrangements of DV-Anl, DV-Anl-DV, DV-Anl-IV, and DV-IV-Anl have been studied. The AFM images show that by applying secondary voltage (direct or inverse voltage), it is possible to drift nanoparticles and change its morphology (size and shape) as well as surface and volume distributions. As a result, by applying a secondary direct voltage (in the DV-Anl-DV case), the surface density of nanoparticles decreases due to direct drift force. It is notable that in this case, the extinction peak and ATR depth have not significantly changed. By applying a secondary inverse voltage (in the DV-Anl-IV, and DV-IV-Anl cases), an increase in the surface density of the nanoparticles has been observed. Also, the extinction peak has increased, and the ATR depth has decreased in the DV-Anl-IV case, but in the DV-IV-Anl case, due to the uniform size of surface nanoparticles, the resonance power has shown a significant increase in both extinction and ATR spectra compared to other cases. The resulting changes in extinction and ATR spectra show that by using the VITAR process, the surface structure, morphology and its optical properties can be optimized and this method provides a great opportunity to enhance Localized Surface Plasmon Resonance (LSPR) effects, which can be employed in nano-optical devices.