In order to make the embryonic form of intragranular structure, the Al2O3/GdAlO3 system was selected due to its excellent mechanical properties. Gd2O3 and Al(NO3)3·9H2O were used as the starting materials. A co-precipitation method was used for the preparation of fine ceramics and applied to synthesize the nano-powder of GdAlO3 firstly. Then, the nano-powder of GdAlO3 was mixed with the precipitates by the second co-precipitation method. After drying and calcination, the compound powder with eutectic composition (77 mol % Al3+—23 mol % Gd3+) was fast sintered by using the spark plasma sintering technique. The results revealed that the phases of the sintered samples were Al2O3 and GdAlO3. The phases showed a homogeneous and interlaced distribution. All the matrix grains were submicron. The sizes of the intragranular structures were between 50 nm and 150 nm. Therefore, the intragranular structure displayed a novel mixture of nanometer–submicron and submicron–submicron types. The different intragranular structures all changed the fracture modes of Al2O3 grains from intergranular fracture to transgranular fracture.