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Mung bean protein hydrolysate has shown some biological properties. Isolated mung bean proteins were hydrolyzed by papain and tested for antiproliferative effects on cancer cells. It was confirmed that the mung bean peptides could inhibit the proliferation of tumor cells in mice, without the side effects of chemical anticancer drugs, and that the mung bean peptides promoted apoptosis of HepG2 cells and arrested the cell cycle in the S phase at a low dose and the G0/G1 phase at a high dose. Subsequently, the hydrolysates were purified through ultrafiltration and Sephadex G-15 gel chromatography. Fraction A, obtained following size-fractionation (<3 kD) and column chromatography (acetic acid elution), showed the highest inhibition of cell proliferation, which was 86.35% at 2.99 mg/mL. UPLC-MS/MS was used to identify four peptides that could inhibit HepG2 cell proliferation: VEG, PQG, LAF and EGA. These peptides mainly contained Glu, Asn, and Gln and the hydrophobic amino acids Gly, Ala, Val and Ile. These results indicated that mung bean protein hydrolysate exhibited both in vitro and in vivo anticancer activities and provided insights into the future development and utilization of mung bean peptides as functional foods with the aim of inhibiting the proliferation of hepatocellular carcinoma cells.