Layered double hydroxide (LDH)-based nanocomposites, constructed by interacting LDH nanoparticles with other nanomaterials (e.g. silica nanoparticles and magnetic nanoparticles) or polymeric molecules (e.g. proteins), are an emerging yet active area in healthcare, environmental remediation, energy conversion and storage. Combining advantages of each component in the structure and functions, hierarchical LDH-based nanocomposites have shown great potential in biomedicine, water purification, and energy storage and conversion. This feature article summarises the recent advances in LDH-based nanocomposites, focusing on their synthesis, structure, and application in drug delivery, bio-imaging, water purification, supercapacitors, and catalysis.