Solar-driven semiconductor-based molecular hydrogen production is an ideal protocol for converting abundant solar energy to green fuel. However, this process suffers from costly semiconductor nanostructures, low efficiency, and poor stability. Here, we design a noble-metal-free photocatalyst, CdS-NiFe layered double hydroxide (LDH) nanocomposite, which is synthesized using the liquid-phase pulsed-laser ablation and hydrothermal method. The nanocomposite has a unique morphology of 2D-NiFe LDH nanosheets on 1D-CdS nanorods. The interfacial contact of heterostructures allows the efficient carrier transport and migration due to the appropriate potentials, which greatly reduce the recombination of carriers. It also provides a significant number of catalytically active sites for the hydrogen evolution reaction due to its thin and flexible nature and high specific surface area. The CdS/NiFe nanocomposite exhibits a hydrogen evolution rate of 72 mmol g–1 h–1, which is higher than reported nanocomposites of CdS-ba...