Tropospheric ozone (O3) is a phytotoxic air pollutant that can impair visible foliar injury (O3 VFI) and reduces photosynthesis in sensitive forest species. Viburnum lantana L. has been widely used as an in situ bioindicator of O3 pollution in mountainous areas of Europe; however, field-observed O3-induced VFI as well as critical levels (CLs) established to protect forests, have not been validated. This study validated field-observed O3 effects in V. lantana through experiments carried out in a Free-air O3 eXposure infrastructure (FO3X) and determined which O3 metric (exposure-based—AOT40 or flux-based—POD1) best explains O3 effect on leaf physiology and VFI. V. lantana saplings were subjected to ambient air (AA) conditions and elevated O3 levels at 1.5× and 2.0× AA. Throughout the experimental period (T1: 2-month and T2: 3.5-month O3 exposure) measurements were taken for the Plant Injury Index (PII), light-saturated net photosynthetic rate (Asat), stomatal conductance (gs), leaf color index (SPAD), and the maximum photochemical efficiency of photosystem II (Fv/Fm). O3 VFI was first observed in 2.0× after 16 days. As a result, O3 treatment influenced PII, which was significantly higher in the 2.0× (9.06 ± 3.24) than in the 1.5× and AA treatments (1.31 ± 0.62 and 1.29 ± 0.71) at T2. The Asat, SPAD, and Fv/Fm were significantly affected by O3 treatments; no significant difference in gs was found. POD1 better explained variability in O3 VFI and physiological parameters, with CLs proposed for V. lantana of 1.61 mmol m–2 and 1.22 mmol m–2 for a 4% reduction of Asat and gs, and a CL of 7.82 mmol m–2 for the onset of O3 VFI.