Molecular orientation control with a template material, perylene 3,4,8,9-tetracarboxylic dianhydride (PTCDA), was investigated for various p-conjugated crystalline molecules, namely copper phthalocyanine (CuPc), N, N'-Dimethyl-3,4,9,10-perylenedicarboximide (MePTC), pentacene and dinaphtho[2,3-b: 2', 3'-f]thieno[3,2-b]thiophene (DNTT). The molecular orientation of CuPc and MePTC clearly changed from edge-on to face-on orientation by depositing on PTCDA. The electron mobility of MePTC, which is an ntype organic semiconductor suitable for vertical carrier transport, improved approximately three times owing to face-on molecular orientation. Thin-film X-ray diffraction studies revealed that the molecular packing mode (stacking or herringbone) affects the molecular orientation control. The MePTC film oriented with PTCDA was applied to a vertical-type organic transistor, a metal base organic transistor (MBOT), resulting in higher output current and current gain. (c) The Author(s) 2019. Published by ECS.