Total phenolic contents (TPC), total flavonoid contents (TFC), related antioxidative and antiradical capabilities of grape cane extracts from 11 varieties (five V. vinifera cultivars and six Chinese wild grapes) widely grown in China were evaluated. Antioxidant properties were determined as DPPH and ABTS radical-scavenging abilities, superoxide anion and hydroxyl radical and hydrogen peroxide scavenging assays, as well as reducing power. Phenolic profiles of the extracts were characterized by using high-performance liquid chromatography (HPLC) techniques. All extracts exhibited strong antioxidant and effective free radical inhibition activities (EC50 values), which generally correlated negatively with TPC (r = −0.804 to −0.918) and TFC (r = −0.749 to −0.888). In comparison with gallic acid, Trolox and tert-butylhydroquinone (positive controls), most grape cane extracts showed more efficient scavenging effects toward different reactive oxygen species. HPLC analysis revealed the presence of (+)-catechin, (−)-epicatechin, and trans-resveratrol as major phenolic components in the extracts. These results suggest that grape cane extracts may serve as a potential source of natural antioxidant for food and pharmaceutical application.