In order to investigate the relationship between nanocomposite hydrogels and polymerizable liquid crystal surfactant, under the physical cross-linking of nanoclay lithium magnesium silicate hydrate (LMSH), a series of poly(NIPAm-LMSH-AAc-Brij-58) nanocomposite hydrogels, based on the copolymerization of polymerizable liquid crystal AAc-Brij-58 synthesized by esterification reaction and N-isopropylacrylamide (NIPAm), were synthesized by in situ free-radical polymerization. The results show that with increasing AAc-Brij-58 concentration from 0 to 1 wt%, the particle sizes decrease from approximately 143 to 60 nm, and the appearance becomes cruciform or flower type and rod shape, respectively. The obtained nanocomposite hydrogels present thin pore walls and larger pore diameters. With increasing mass ratios of AAc-Brij-58/NIPAm from 0 to 1/15, the maximum swelling ratios exhibit an increasing tendency, the volume phase transition temperatures increase from 32.10 to 33.56 °C, and thermal degradation temperature increase from 305 to 340 °C.