0–3 (Pb[(Mn1/3Nb2/3)1/2(Mn1/3Sb2/3)1/2]0.04(ZrxTi1-x)0.96O3)(PZT)/carbon black/Poly (vinylidene fluoride) (PVDF) pyroelectric composites were prepared by hot-pressing technology. The volume conductivity, specific heat capacity, dielectric, piezoelectric and pyroelectric properties of the composites with various nano carbon black powder contents were discussed. The results showed that the nano carbon black powder acted as a conductive phase which could improve the conductive of the composites, thereby enhance the electrical properties. With addition of 0.9 wt% nano carbon black powder, the composites exhibited the best pyroelectric property, which was about 1.3 times of those composites without nano carbon black powder. It is concluded that nano carbon black powder doping is an effective method to improve the pyroelectric performance of the composites, which is good candidate for the future infrared detector application.