Nerium oleander L. is a widely used medicinal plant for pharmaceutical purposes. In this work, an extract of the pink flowers of this plant (FE) was characterized in terms of phenolic composition by LC-DAD-ESI-MS/MS and bioactivity, namely, antioxidant and antiproliferative effects. A total of 20 compounds from different classes, including derivatives of phenolic acids and flavonoid glycosylated derivatives, were identified in FE. Chlorogenic acid was the dominant phenolic compound in the extract (62.28 ± 1.74 μg mg⁻¹ of dry extract). The antioxidant activity was assessed by ORAC assay, and FE showed an ability to reduce peroxyl radicals (ORAC value of 791.26 μmol TEAC per g DE). Additionally, the FE inhibited the proliferation of a colorectal cancer cell line (HT29 cells, EC₅₀ = 11.72 ± 0.02 μg mL⁻¹) and showed no cytotoxicity to confluent Caco-2 cells, a model of human intestinal epithelium. These results provide new information about the phenolic composition of Nerium oleander pink flowers and the bioactivity of the extracts.