Neuromodulation induced by transcranial electric stimulation (TES) exhibited promising potential for clinical practice. However, the underlying mechanisms remain subject of research. The combination of TES and electroencephalography (EEG) offers great potential for investigating these mechanisms and brain function in general, especially when performed simultaneously. In conventional applications, the combination of EEG and TES suffers from limitations on the electrode level (gel for electrode-skin interface) and the usability level (preparation time, reproducibility of positioning). To overcome these limitations, we designed a bifunctional cap for simultaneous TES–EEG applications. We used novel electrode materials, namely textile stimulation electrodes and dry EEG electrodes integrated in a flexible textile cap. We verified the functionality of this cap by analysing the effect of TES on visual evoked potentials (VEPs). In accordance with previous reports using standard TES, the amplitude of the N75 component was significantly decreased post-stimulation, indicating the feasibility of using this novel flexible cap for simultaneous TES and EEG. Further, we found a significant reduction of the P100 component only during TES, indicating a different brain modulation effect during and after TES. In conclusion, the novel bifunctional cap offers a novel tool for simultaneous TES–EEG applications in clinical research, therapy monitoring and closed-loop stimulation.