Blackberries have high nutritional value and strong biological activities, such as antiproliferative activity. Anthocyanins are important functional components in blackberries. We collected 25 kinds (lines) of blackberries from our nursery to investigate antiproliferative agents in natural foods. Among them, the Shuofeng variety had the highest anthocyanin content, with 2.54 mg/g of fresh fruit, which increased to 357.75 mg/g of dried powder through ultrasound-assisted solvent extraction and macroporous resin adsorption. Additional experiments showed that Shuofeng’s anthocyanin content had high anti-HepG2 activity in vitro and in vivo, as well as activity against Hela (68.62 μg/mL), HepG2 (55.85 μg/mL), MCF-7 (181.21 μg/mL), and A549 cells (82.01 μg/mL), as determined by MTT assay. It also had no apparent toxic effects. The combination of DDP and DOX significantly enhanced the antiproliferative activity of the four cell lines. The IC50 value of Shuofeng’s anthocyanin content combined with DOX in HepG2 cells was the lowest at only 0.08 μg/mL, indicating that the combination of drugs had additive and synergistic effects. Shuofeng’s anthocyanin content might intercalate into DNA and alter or destroy DNA, causing apoptosis and inhibiting cell proliferation. Our results show that blackberry anthocyanins can inhibit the proliferation of cancer cells and their possible mechanisms. However, we must study the deeper mechanism and explore its targeting effects in the future.