The ordered L12-type Al3Ti–(8, 10, 15)% Cr intermetallic compounds, namely, Al67Ti25Cr8, Al66Ti24Cr10, and Al59Ti26Cr15, were prepared by induction melting followed by thermomechanical treatment. Their microstructure, compositional variation, and crystal structure were characterized using X-ray diffraction, optical microscopy, and scanning and transmission electron microscopy equipped with energy-dispersive spectroscopy. The Al67Ti25Cr8 alloy consisted of the L12-Al3Ti matrix and precipitates of α2-Ti3Al, D022-Al3Ti, and γ-TiAl. The Al66Ti24Cr10 and Al59Ti26Cr15 alloys consisted of the L12-Al3Ti matrix and grains of α-TiAl and β-Cr.