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The reduction in particle size of ZnO pellet in the nanoscale range was achieved using a hybrid thermo-vibrational annealing and dry-quenching set-up, which was designed and fabricated in-house and is simple and low-cost to operate. Initially, ZnO pellets were synthesized through pyrophoric method and then annealed at 8000C in this processing device. To confine grain growth during the recrystallization stage of annealing, vibrational energy was applied during annealing and dry-quenching to cool. This step-by-step post-synthesis technique involves the simultaneous application of thermal and mechanical vibrational energy to the ZnO pellet for 4 hours, followed by vibrational-dry quenching. Both annealed pellets, i.e., ZnO annealed without vibration and ZnO annealed with vibration, were studied using XRD, SEM, HRTEM, FTIR, UV-Visible, and Raman spectroscopy to conduct a comparative investigation of various structural, microstructural, and optical properties. Although both ZnO pellets had polycrystalline hexagonal wurtzite structures without any secondary phases, the average crystallite sizes of ZnO pellets with vibration were smaller than those without vibration, which were 36.566nm and 25.308nm, respectively, according to the XRD data. Analysis using SEM and HRTEM yielded similar confirmatory results. FTIR and Raman examinations revealed the presence of various functional groups and vibrational modes, which were confirmed by experimental results. The greater optical bandgap of 3.36 eV seen in the UV-Visible spectra of the ZnO with vibration sample indicates that it is a promising material for the creation of enhanced electrical, optoelectronic, and sensor devices based on ZnO nanoparticles, among other applications.