Ten phyllospheric yeast strains were studied for their potential as biocontrol agents against fruit spoilage mould. The efficacy of these yeasts against Botrytis cinerea and Fusarium fujikuroi was assessed using dual-culture, mouth-to-mouth, radial growth inhibition and post-harvest fruit assays. Additionally, their capacity for producing hydrolytic enzymes was examined. Results from the ten yeasts revealed dual culture antagonism ranging from 41% to 63% against B. cinerea and 23% to 48% against F. fujikuroi, along with radial inhibition ranging from 70% to 100% and 47% to 100%, respectively. Additionally, in vitro inhibition through the production of volatile organic compounds (VOCs) varied from 2% to 46% against B. cinerea and 6% to 64% against F. fujikuroi. Overall, Aureobasidium melanogenum J7, Suhomyces pyralidae Y1117, Dekkera anomala V38, and Rhodotorula diarenensis J43 emerged as the best-performing biocontrol yeasts. Volatile organic compounds produced by the four yeasts were also identified and included in fruit bioassays using pears and tomatoes. Various VOCs, including 1-butanol, 3-methylbutanol, and butyric acid, were linked to the antagonistic properties of the selected yeasts. Lastly, the four chosen yeast strains significantly mitigated post-harvest spoilage caused by B. cinerea and F. fujikuroi in pear and tomato fruits, with D. anomala V38 exhibiting the greatest inhibitory activity. These findings underscore a potential sustainable and efficient approach to reducing mould-induced post-harvest spoilage while reducing reliance on synthetic fungicides.