Bulk Zr60Cu20Pd10Al10 amorphous alloy was rolled at room temperature up to 96% reduction in thickness without fracture. The changes of microstructure and hardness during rolling deformation were investigated by X-ray diffraction, differential scanning calorimetry, high-resolution transmission electron microscopy, and microhardness measurement. It is revealed that the rolling deformation causes the quenched-in nuclei in the glass to grow slowly before a deformation degree of 90%. Substantial nanocrystallization occurs at higher deformation degree, where the softening induced by shear bands can even be compensated by the nanocrystallization.