The dependence of pentacene nanostructures on gate dielectric surfaces were investigated for flexible organic field-effect transistor (OFET) applications. Two bilayer types of polymer/aluminum oxide (Al(2)O(3)) gate dielectrics were fabricated on commercial Al foils laminated onto a polymer back plate. Some Al foils were directly used as gate electrodes, and others were smoothly polished by an electrolytic etching. These Al surfaces were then anodized and coated with poly(alpha-methyl styrene) (PAMS). For PAMS/Al(2)O(3) dielectrics onto etched Al foils, surface roughness up to approximately 1 nm could be reached, although isolated dimples with a lateral diameter of several micrometers were still present. On PAMS/Al(2)O(3) dielectrics (surface roughness >40 nm) containing mechanical grooves of Al foil, average hole mobility (mu(FET)) of 50 nm thick pentacene-FETs under the low operating voltages (|V| < 6 V) was approximately 0.15 cm(2) V(-1) s(-1). In contrast, pentacene-FETs employing the etched Al gates exhibited mu(FET) of approximately 0.39 cm(2) V(-1) s(-1), which was comparable to that of reference samples with PAMS/Al(2)O(3) dielectrics onto flat sputtered Al gates. Conducting-probe atomic force microscopy and two-dimensional X-ray diffraction of pentacene films with various thicknesses revealed different out-of-plane and in-plane crystal orderings of pentacene, depending on the surface roughness of the gate dielectrics.