Zirconia-supported vanadium–copper catalysts (VCux:yZr) were used for the oxidative depolymerization of softwood LignoBoost Kraft lignin (LB). Various VCux:yZr catalysts were prepared (x:y = 0:1, 1:4, 1:2, 3:4, 1:1, and 1:0) by incipient wetness impregnation, and reactions were performed in alkaline water at 150 °C under an O₂ pressure of 5 bar for 10 min. ¹H–¹³C HSQC NMR spectroscopy was used for product identification and quantification. The most promising catalyst was VCu1:2Zr, giving a total monomer yield of 9 wt% and the highest selectivity for vanillin (59%). This catalyst was characterized before and after use by N₂ physisorption, XRD, TGA, SEM-EDS, and XPS. Cleavage of the main interunit linkages in LB, including the β-O-4 bonds and recalcitrant C–C bonds, was also observed. The findings of this study demonstrate the potential of the V–Cu/ZrO₂ catalyst system in the production of value-added aromatics from technical lignin under relatively mild conditions. This would contribute to the more sustainable use of an underutilized side-stream in forest-based industries, provided catalyst reuse can be successfully demonstrated.