The effect of high pressure on the microstructure of annealed amorphous Nd9Fe85B6 alloy was studied. It was found that application of high pressure made the microstructure of the crystallized alloy much more homogeneous. The average grain size of the Nd2Fe14B phase decreased with the increase of pressure, whereas, the size of the α-Fe first increased when a pressure of 1 GPa was applied and then decreased with further increase of pressure. Pressure-induced (410) texture of the Nd2Fe14B phase was also observed. The present study suggested an effective route for controlling the microstructure in a nanoscale solid.