The second harmonic wavelength of a neodymium-doped yttrium-aluminum-garnet (Nd-YAG) laser (λ=532 nm) was used in a pulsed laser ablation technique (PLAL) to synthesize aluminum nanoparticles suspended in white vinegar from an aluminum target. The nanoparticles were characterized by HRTEM and UV-Vis spectrophotometry. They were found to range in size between 2 and 50 nm in diameter, with an average diameter of 12±9 nm. The nanoparticles had a maximum absorption peak at 237 nm and were found to exhibit a core-shell structure with an Al core coated by a thin layer of an amorphous material which could be attributed to amorphous carbon. HRTEM results revealed that the small nanoparticles (<20 nm) had an fcc phase of aluminum crystalline structure, where the larger particles represented alumina (γ-Al2O3) nanoparticles. Such observation suggests that the use of white vinegar as an ablation medium could facilitate the synthesis of aluminum nanoparticles with minimal evidence of the existence of aluminum oxide nanoparticles in the resultant suspension.