A good way to make carbon materials was presented in low-temperature polyvinyl chloride (PVC) carbonization by catalysis. The process of low-temperature PVC carbonization by CuAl-layered double hydroxide (CuAl-LDH) was investigated by thermogravimetric analysis (TGA) and tubular furnace. The results show that CuAl-LDH accounting for 5% of PVC mass enabled acceleration of the dehydrochlorination in PVC as soon as possible and maximized the yield of the PVC carbonized product. The vacuum with 0.08 MPa, 20 °C/min heating rate and 90 min carbonized maintenance time were optimal for PVC carbonization. Moreover, the best morphology and yield of the carbonized product was provided at a carbonization temperature of 300 °C.