Al2TiO5 has received widespread attention due to its lower thermal conductivity in materials with a low coefficient of thermal expansion. Therefore, white fused corundum, tabular corundum and micro α-Al2O3 were selected as alumina sources to prepare Al2TiO5 by in-situ synthesis in this paper. The influence of alumina sources on the phase compositions, microstructure and thermal conductivity of the samples was investigated. The mechanism of the in-situ synthesis of Al2TiO5 was discussed in detail. The results showed that increasing the sintering temperature was beneficial for the formation of Al2TiO5. Besides, adding white fused corundum or tabular corundum was conducive to the preparation of Al2TiO5. The liquid phase formed by a small number of impurities in the raw materials at high temperatures could accelerate the diffusion velocity of Al3+ and Ti4+, which was beneficial to the formation of Al2TiO5 and the stability of its structure. The sample with tabular corundum sintered at 1600 °C had the highest content of Al2TiO5 about 86 wt%, and the largest average grain size of 35.3 μm. It also showed satisfactory performance, with the bulk density of 2.99 g/cm3 and the compressive strength of 98.5 MPa. Moreover, the thermal conductivity at 900 °C was reduced to 0.96 W/(m·K) compared to the sample without tabular corundum, which could be used to prepare Al2TiO5 ceramics with lower thermal conductivity.