Cofiring behavior of composites consisting of ferroelectric PMZNT and ferromagnetic NiCuZn ferrite was investigated via X-ray diffractometer (XRD), thermomechanical analysis (TMA) and scanning electron microscopy (SEM). Mismatch of sintered camber consisting of two layered structure of ferroelectric PMZNT and NiCuZn ferrite was observed. Mismatched sintering behavior was modified by adopting PMZNT and NiCuZn powders to form composite materials. The temperature of appearance pyrochlore phase in prepared composite materials is lower than that of sintering pure PMZNT material. The grain size of PMZNT and NiCuZn in prepared composites is smaller than that of sintering pure PMZNT and NiCuZn ferrite, respectively.