Semiconductor-graphene oxide-based surface-enhanced Raman spectroscopy substrates represent a new frontier in the field of surface-enhanced Raman spectroscopy (SERS). However, the application of graphene oxide has had limited success because of the poor Raman enhancement factors that are achievable in comparison to noble metals. In this work, we report chemical SERS enhancement enabled by the application of an electric field (10-25 V/mm) to aligned semiconducting peptide nanotube-graphene oxide composite structures during Raman measurements. The technique enables nanomolar detection sensitivity of glucose and nucleobases with up to 10-fold signal enhancement compared to metal-based substrates, which, to our knowledge, is higher than that previously reported for semiconductor-based SERS substrates. The increased Raman scattering is assigned to enhanced charge-transfer resonance enabled by work function lowering of the peptide nanotubes. These results provide insight into how semiconductor organic peptide nanotubes interact with graphene oxide, which may facilitate chemical biosensing, electronic devices, and energy-harvesting applications.