Poly(gamma-benzyl L-glutamate) (PBLG) was bonded covalently to a flat substrate, and it formed an aligned dipole layer (PBLG-CRA film). Using the PBLG-CRA film as an orienting film for a nematic hydrogen-bonded liquid crystalline complex, 60BA-9Py (formed from 4-(hexyloxy)benzoic acid (60BB) and 4-nonylpyridine (9Py)), complexes, not only in the vicinity of the CRA film but also in the bulk layer, were able to respond more rapidly to an applied electric field when using a rubbed polyimide film, and they became responsive at frequencies in the MHz region. We conclude that the PBLG-CRA film has a dynamic orienting force, that dipole-dipole interaction takes place between the interfacial 60BA-9Py complexes and the PBLG molecules, and that the movement of the interfacial 60BA-9Py complexes is smoothly transferred to the bulk layer because the electric state of the complex 60BA-9Py in the bulk changes under the influence of the CRA film.