This study was designed to evaluate the chemical composition, buffer N solubility, in vitro ruminal N degradation and in vitro ruminal biological activity of condensed tannins in Acacia erioloba, Acacia nilotica and Ziziphus mucronata leaves harvested from two sites (Masuthle communal grazing land and Molelwane private farm). Leaves were harvested, dried at 60 °C and milled. The highest crude protein (CP) content was found in leaves of Z. mucronata (177.7 g/kg DM). Leaves harvested from Masuthle had higher (p < 0.05) soluble phenolics (SPh) (44.6 g TAE/kg DM) compared to those harvested from Molelwane (29.8 g TAE/kg DM). In both Molelwane and Masuthle, leaves of A. nilotica had higher levels of condensed tannins (CT) (0.76 AU550/200 mg and 0.52 AU550/200 mg respectively) followed by A. erioloba and Z. mucronata, which did not differ (p > 0.05). Nitrogen degradability at 24 h was the same (p > 0.05) for all tree species but not at 12 and 36 h. No linear association (p > 0.05) was found between buffer-soluble N and in vitro ruminal N degradability in leaves with high SPh content. The largest polyethylene glycol (PEG) effect was in leaves of A. nilotica (448%) harvested from Masuthle after 36 h of incubation. Ziziphus mucronata leaves harvested from Molelwane had the least PEG effect at 48 h. There was no linear association (p > 0.05) between PEG effect and SPh for all incubation periods, but a positive relationship was observed between PEG effect and condensed tannins content. There was no linear association between solubility index (SI) and in vitro ruminal N degradability for tannin-rich leaves. It was concluded that higher browsing pressure in Masuthle communal rangeland resulted in leaves with higher levels of condensed tannins, which had higher in vitro ruminal biological activity, compared to those harvested from Molelwane.