The fourth-order coherent Raman response of a TiO<sub>2</sub> (110) surface covered by HCl aqueous solution, neat octanol, acetic acid, or carbon tetrachloride layers is acquired. Four fourth-order optical responses were identified at 837–826, 452–448, 371–362, and 184–183 cm<sup>−1</sup> and assigned to near-surface phonons of TiO<sub>2</sub>. A third-order response produced in the bulk liquid layer was superimposed on the fourth-order response, when coherent vibrations are efficiently excited in the layer.
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