A selectively doped InP/In0.53Ga0.47As heterostructure has been prepared by chloride transport vapor phase epitaxy. Hall and Subnikov‐de Haas measurements revealed the existence of a high mobility, two‐dimensional electron gas at the interface of this heterostructure. Enhanced electron mobilities were as high as 106 000, 71 200, and 9 400 cm2/Vs at 4.2, 77, and 300 K, respectively. These indicate the excellent interface properties of the selectively doped InP/In0.53Ga0.47As heterostructure grown by chloride transport vapor phase epitaxy.