Nanoscale NiAl-NO3-LDHs with good crystallinity have been synthesized by a method, Separate Nucleation and Aging Steps (SNAS). An NiAl-NO3-LDHs/LDPE composite was prepared by blending NiAl-NO3-LDHs and LDPE in a heated double-roller mixer. The color of this composite changed from olive green to steel gray under UV irradiation. After heating at 80℃ for 2 h, the color returned to olive green. The effect of varying the amount of added NiAl-NO3-LDHs and UV exposure time on the photochromic properties of the composite has been investigated. The results showed that the photochromic phenomenon becomes more apparent with increasing amount of NiAl-NO3-LDHs. When the amount reaches 5%, the composite exhibits good photochromic properties and reproducibility. The color change rate of the composite reaches a maximum when the irradiation time exceeds 20 min. The addition of LDPE improves the photochromic cyclability of NiAl-NO3-LDHs significantly. The addition of nanoscale NiAl-NO3-LDHs also improves the mechanical properties of LDPE to some extent.