A dual-functional coating with both superhydrophobic and UV-blocking properties was prepared on cotton fabric using a hybrid layered double hydroxide (LDH) nanoplatelet intercalated with 2-hydroxy-4-methoxybenzophenone-5-sulfonic acid (HMBS) molecules and an electrostatic layer-by-layer (LbL) assembly technique. The thermal stability of HMBS was greatly enhanced by the host–guest interaction with LDH layers. The as-prepared HMBS@LDH hybrid had a nearly neutral surface charge. To make it carry enough charge for the electrostatic LbL assembly, the HMBS@LDH nanoplatelet was further modified with 3-aminopropyltriethoxy silane. The nanoscale roughness generated by LDH nanoplatelets, together with low-surface-energy fluoroalkylsilane, endowed cotton fabrics with superhydrophobicity. The HMBS@LDH coating showed up to four-fold increase in the UV protection ability of cotton fabrics