We report the growth and characterization of ultrapure InP using trimethylindium and phosphine by atmospheric pressure organometallic vapor phase epitaxy (APOMVPE). The 77 K mobility of 131 000 cm2 /V s is the highest ever obtained by APOMVPE and among the highest ever measured for InP using any growth technique. The low‐temperature photoluminescence measurements reveal that impurity reduction occurs at higher growth temperatures.