Initial powders of Zr, Al, C and Zr, Al, ZrC were used for the synthesis of MAX phases of the compositions Zr2AlC and Zr3AlC2. The highest content (50.4 vol %) of the MAX phase Zr3AlC2 was obtained using the initial powders Zr/Al/ZrC in the ratio of components 1 : 1.5 : 2 with the addition of 5 vol % of Al. The optimal temperature for the synthesis of a material based on the MAX phase Zr2AlC is 1525°C, and that of the material based on Zr3AlC2—1575°C. The structure of the synthesized MAX materials includes elongated grains of the compositions Zr2AlC and Zr3AlC2, which determines their high strength. Zirconium carbide, as an intermediate phase, is always present in the final products. Due to the considerable evaporation of aluminum, the ZrO2 phase is also present in the synthesis products. Excess aluminum contributes to the maximal formation of Zr2AlC and Zr3AlC2 phases during synthesis.