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How to obtain a large sensitivity has been a central issue of lateral photovoltaic effects (LPEs) since it had been discovered many decades ago. This work reports a colossal LPE in a nanolayer Ti and TiO2 modulated metal-oxide-semiconductor (MOS) structure of Ti/TiO2/Si. The obtained 169 mV/mm sensitivity in this structure represents currently the highest level compared with previously reported results of 700 μV/mm-60 mV/mm in any other systems. The results indicate this MOS structure can be used as novel position-sensitive detectors with high sensitivity.