The Al3Ti intermetallic compound was fabricated with pure Ti powder and aluminum plate as starting materials by self-developed rotational extrusion equipment. The microstructure of the rotational extrusion alloyed product was observed with scanning electron microscopy and energy dispersive spectrometry, the phase constituent of alloying product was inspected by transmission electron microscopy and X-ray diffraction, and the microhardness was measured. The results show that under the interaction effect of the friction stick shearing and extrusion force, the Ti-Al intermetallic compounds can be synthesized by alloying reaction, and the product is Al3Ti phase intermetallic compound. The size of Al3Ti particles is about 500 nm, and the matrix of aluminum presents a large number of dislocations, which are irregular arrangement of curly state. The average microhardness of alloyed product is 1080 MPa, four times that of matrix.