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The effects of directional solidification parameters and the coupling of directional solidification parameters and alternating electromagnetic fields on separation and enrichment of the C54–TiSi2 phase were investigated in a directionally solidified hypoeutectic Ti–65 wt.％ Si alloy. The results indicated that by increasing the pull-down velocity at a given position within the ingot, the cooling rate, growth rate, and temperature gradient of ingot could be increased. At a pull-down velocity near 5 μm/s, the temperature gradient, cooling rate, and growth rate decreased with increasing the thickness of the C54–TiSi2-rich layer. Electromagnetic fields enhanced mass transfer at pull-down velocities of 5, 10, 15, and 20 μm/s, with resulting enriched layer thicknesses of 15, 10, 10, and 5 mm, respectively. By increasing the percentage of Ti in the Ti–Si alloy from 25 to 35 wt.％, the thickness of the C54–TiSi2-rich layer was increased from 2.5 to 3.3 cm. However, the maximum C54–TiSi2 content obtained experimentally in this layer decreased from 92.06 to 79.49 mass％.