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Ce-based materials have gained considerable prominence in catalysis as a type of the most valuable material for various applications ranging from automotive emission control to CO2 and water splitting. We here report a novel type-II CeO2/CeF3 composite, composed of two paradigms of Ce-based binary compounds, prepared by a facile one-step in-situ hydrothermal method, and explore its potential as a photocatalyst for solar energy conversion. Primarily, the morphologies, particle size and microstructures of CeO2/CeF3 composite can be modulated by the volume ratio of ethanol to water in the precursor solution. The photocatalytic activities firstly increase to a maximum and then decrease with the increased amount of ethanol. The hybrid CeO2/CeF3 particles with large size and polyhedron morphology exhibit superior photocatalytic activity, having a high rate constant k of MB decomposition about 7.6 times faster than that of the lowest one. A multiple synergetic mechanism in CeO2/CeF3 composite, which is featured by obvious promoted separation of photogenerated electrons and holes at the type-II heterojunction interfaces and in particular between the different facets of microcrystals, and the highly reactive facets exposed, has been proposed to account for its distinguished photocatalytic activity. This work provides some new insights for the synthesis and optimization of novel rare earth Ce-based composite photocatalyst with high photocatalytic performance.