The beneficial effects of walnuts and walnut products on human health, due primarily to their rich polyphenolic content, have been appreciated as an empirical fact for centuries. The purpose of this study is to determine the polyphenolic contents of liqueurs made from the walnut selections ‘Rasna’ and ‘Sava’ and the walnut cultivar ‘Šampion’ (all harvested at three different times), as well as the polyphenolic contents of their green husks. The walnut liqueurs were prepared according to two traditional recipes using young walnut fruits. The highest antioxidant capacity was recorded in the liqueur made from the ‘Rasna’ walnut selection (89.94%), whereas the highest contents of phenols (83.28 mg GAE/g FW), flavonoids (0.83 mg QE/g FW) and proanthocyanidins were found in the liqueur made from the ‘Šampion’ cultivar (14.75 mg CE/g FW). The youngest ‘Rasna’ walnuts, harvested at the first experimental time point, exhibited the highest phenolic and tannin contents, whereas the highest flavonoid content was observed in the ‘Šampion’ cultivar. The biochemical results obtained indicate a decrease in the polyphenolic content of walnut fruits with their growth and development. Moreover, the polyphenolic profiles of the walnut liqueurs considered were found to be greatly affected by the method of preparation and the cultivar/selection of walnuts.