Geranium robertianum L. has been used in folk medicine and herbalism practice for the treatment of various conditions, but the study of its bioactivity has been barely addressed. Although its phytochemical composition has received some attention, contributions to the nutritional composition are practically unknown. Herein, G. robertianum gathered in Trás-os-Montes, Northeastern Portugal, was chemically characterized regarding nutritional parameters, and the antioxidant activity and cytotoxicity against several human tumor cell lines and non-tumor porcine liver primary cells of several aqueous and organic extracts were evaluated. G. robertianum showed to be an equilibrated valuable herb, rich in carbohydrates and proteins, and poor in fat, providing sugars, tocopherols, organic and essential fatty acids. Amongst the extracts, the acetone one showed the highest total phenol and total flavonoid contents, as well as the greatest antioxidant and cytotoxic activities. This extract showed to contain hydrolysable tannins (e.g. geraniin and castalagin/vescalagin), as the main phenolic compounds.