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In operando nuclear magnetic resonance (in operando NMR) was used to investigate the effects of co-catalysts and wavelength of light on the products of photocatalytic methanol reforming, as well as the hydrogen production rate, in a real solid-liquid reaction environment. The results demonstrated that adding co-catalysts (i.e., anatase TiO2 modified with different isolated noble metal atoms) could affect the yields of reforming products to some extents, but had only little effects on the reaction kinetics. And the wavelength of light also had a large effect on the yields. It was concluded that the co-catalysts might play important roles in providing the redox capacity and the synergistic effects between methanol oxidation and hydrogen production.