We investigated the orbital anisotropy of GaFeO3 using the Fe L2,3-edge x-ray magnetic circular dichroism and the polarization dependent O K-edge x-ray absorption spectroscopy. We found that the system shows a considerably large orbital momentum and anisotropic Fe-O bonding, which are unexpected in a half-filled d5 system such as GaFeO3. The orbital and bonding anisotropies, which turn out to be induced by the lattice distortions with exotic off-centering site movements, contribute the large magnetocrystalline energy and magnetoelasticity. These results provide critical clues on the microscopic understanding of the magnetoelectricity.