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It has been rarely reported the morphological control of derivatives of metal‐organic frameworks (MOFs) in hydrothermal conditions for photocatalytic applications. We report here a family of highly efficient composite photocatalysts composed of terephthalic acid/terephthalate (TPA) ligand and TiO₂with various morphologies (e. g., nanoparticles, nanosheets, and nanorods). The composites are synthesized by a simple one‐step hydrothermal method in various solvents (i. e., H₂O, HF, H₂SO₄, HCl, and HNO₃) using Ti‐based MOF (MIL‐125(Ti)) as precursor. The formation mechanism of composite materials with different morphological features is discussed. Impressively, the composite of TiO₂nanoparticles/TPA synthesized using H₂O as solvent under hydrothermal condition exhibits the highest photocatalytic H₂activity among the studied materials, with a photocatalytic H₂production rate of 6.38 mmol g⁻¹ h⁻¹, which is approximately 7.5‐fold higher than pure TiO₂(Degussa, P25) and prominent apparent quantum efficiency (AQE) of 65 % at 365 nm. Furthermore, the mechanism of boosted photocatalytic H₂production is discussed.