The anisotropy of hybrid composite such as Al/GFRP laminates made it possible to control the fiber orientation according to the loading patterns. Therefore, it is important to study the fatigue and delamination behaviors of Al/GFRP laminates by fiber orientation. Al/GFRP laminates of three different fiber orientations (0°, 45°, 90°) were chosen, and the progressive delamination behavior was examined through the fatigue tests. The effects of the fiber orientation on the crack length, the fatigue life, the delamination, the crack growth rate (da/dN), and the stress intensity factor range ( ΔK) were investigated and discussed. The findings led to a conclusion that the effect of fiber orientation should not be ignored in analyzing the progressive damage of Al/GFRP laminates.