Both the particle size and compositions have a strong influence on the UV-shielding performance of layered double hydroxides (LDHs), and they will interact with each other. To investigate the effects of divalent metal ions on the UV-shielding properties of layered double hydroxides (LDHs), MII/MgAl-CO3 LDHs (M = Mg, Co, Ni, Cu, or Zn) with the same primary and secondary particle size have been prepared and their UV-shielding performance have been studied in this work. The UV-vis spectra show that the ZnMgAl-LDHs exhibit the highest absorbance under the ultraviolet B and ultraviolet A rays among these LDH samples, but in the ultraviolet C region, the CuMgAl-LDHs show the highest absorbance and this result is in good accordance with the UV-shielding performance, which was examined by protecting the photocatalytic degradation of rhodamine B aqueous solution. Moreover, under UV rays, PP/ZnMgAl-LDH films show excellent resistance to UV aging, which can be attributed to the strong inhibition of ZnMgAl-LDHs during the production of free radicals in polypropene, as has been confirmed by electron spin resonance results.