Geranium robertianum L., commonly known as Herb Robert, is an herbaceous plant popularly known for its functional properties including antioxidant and anti-inflammatory activities. In this study, the phenolic profile of leaf and stem decoctions of Geranium robertianum L. was elucidated by UHPLC-DAD-ESI-MSn analysis, and their antioxidant and anti-inflammatory potentials were assessed in vitro. Importantly, and envisaging the use of these extracts in human diets, the potential toxicity of bioactive concentrations was also addressed in macrophages and hepatocytes. Both extracts revealed high amounts of ellagitannins, although a slight prevalence of these compounds was observed in that originating from leaves. High radical scavenging activities against DPPH˙, ABTS˙+ and OH˙ were observed either for the leaf or the stem extract, as well as good activities towards ferric reducing antioxidant power, lipid peroxidation and oxygen radical absorbance capacity. In addition, both extracts were very effective at scavenging NO˙, as measured in a chemical model, while only the stem extract was able to decrease the production of this radical by stimulated macrophages. On the other hand, none of the extracts was able to modulate the activity of lipoxygenase or the expression of the inducible nitric oxide synthase. Overall, these data allowed us to conclude that G. robertianum L. stem and leaf decoctions are particularly rich in tannins. The strong scavenging effects displayed by the stem extract suggest that its anti-inflammatory activity may partially result from its anti-radical capacities towards NO˙.