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Abstract Photoresponsive molecules have been widely applied to solar cells and molecular devices. In this manuscript, we report the photoresponsive behaviours of chlorophosphonazo III, a cheap commercially available molecule and previously only used as a colorimetric reagent for earth metals, focusing on the photoisomerization properties in solution or on TiO 2 substrates. Apart from the optomechanical properties, the chlorophosphonazo dye is found to generate a weak but non-negligible photocurrent under the visible light in aqueous environment. Density functional theory calculations are used to understand the structural, electronic and optical properties of the functional molecule. Possible routes to enhance the optoelectronic and optomechanical performance of chlorophosphonazo III toward multiple functions in integrated devices where both of the optomechanical and optoelectronic performances are desired are suggested. Highlights • Photoresponsiveness of chlorophosphonazo III are reported. • It generates a very weak but non-negligible photocurrent. • The interplay between the photoresponsiveness is explained. [ABSTRACT FROM AUTHOR]