To address the pressing demand for hyphenated in situ characterization of the electrode-electrolyte interfaces at the molecular level, we report herein a technical note to demonstrate the hyphenation of in situ electrochemical surface-enhanced infrared absorption spectroscopy (SEIRAS) and shell-isolated nanoparticle enhanced Raman spectroscopy (SHINERS). The core setup incorporates a top-down configured Raman optic fiber head loaded on a 3-dimension positioning module and a bottom-up configured attenuated total reflection infrared spectroscopy (ATR-IR) spectroelectrochemical cell accommodated in a custom-designed optical accessory. The feasibility of this integrated design is initially validated by the simultaneous measurement of two model systems, namely, potential dependent adsorption of pyridine on a Au film electrode and the CO2 reduction reaction on a Cu film electrode by in situ SEIRAS and SHINERS, yielding distinct and complementary spectral information.