Layered double hydroxide (LDH) is a class of 2D nanomaterials, which endows auspicious properties for ameliorating the photocatalytic performance in the realm of solar‐to‐chemical production stemming from the chemical versatility of their host layers. However, pristine LDH suffers from slow charge‐carrier mobility, high rate of electron–hole recombination as well as a tendency to agglomerate, rendering them unbefitting for practical use. Due to the aforementioned bottlenecks, structural modifications such as thickness tuning, cocatalyst incorporation, semiconductor coupling, and ternary heterostructure engineering have been extensively investigated to elucidate a new lease of landscape to the burgeoning potential of LDHs toward artificial photosynthesis. This review summarizes a panorama of state‐of‐the‐art advancements related to the synthesis and modification of LDH‐based nanocomposites for enhanced physicochemical properties toward boosted photocatalysis. Particularly, their progress in versatile energy applications in photocatalytic water splitting (hydrogen and oxygen evolution), and nitrogen and carbon dioxide reduction reactions will be systematically presented. Insights into band structures, electronic properties, and charge‐carrier dynamics of LDH‐based nanostructures will be discussed to unravel the structure–performance relationship. Finally, this review will prospect the invigorating prospectives and opportunities in engineering next‐generation LDH‐based photocatalysts with augmented performances to pave new inroads at the forefront of this research.