We studied the influence of misorientation angles and directions of single crystal diamond (111) substrates on the surface morphology of homoepitaxial diamond (111) films grown by microwave plasma‐enhanced chemical vapor deposition (CVD) in the anisotropic lateral growth mode. Hillocks were completely suppressed on the diamond (111) films grown by CVD on the substrates with misorientation angles of 2° and 4°, while hillocks were formed on the CVD‐grown diamond (111) films on the substrates with misorientation angles of 0° and 1°. In addition, an atomically flat diamond (111) film was grown on the substrate with a misorientation angle of 2° toward the true〈true1¯true1¯2true〉 direction, while rough films were grown on the substrate with a misorientation angle of 2° toward the 〈11true2¯〉 direction.