We report on the formation mechanism of large Schottky barrier height (SBH) of nonalloyed Cr Schottky contacts on strained Al0.25Ga0.75N/GaN. Based on the current-voltage (I-V) and capacitance-voltage (C-V) data, the SBHs are determined to be 1.98 (±0.02) and 2.07 (±0.02) eV from the thermionic field emission and two-dimensional electron gas (2DEG) calculations, respectively. Possible formation mechanism of large SBH will be described in terms of the formation of Cr-O chemical bonding at the interface between Cr and AlGaN/GaN, low binding-energy shift to surface Fermi level, and the reduction of 2DEG electrons.