MnZn ferrite/Permalloy composites have potential in high frequency magnetic applications and can be made into thick-film devices by air plasma spray. The as-sprayed composites have lower saturation magnetization than the starting powder. After annealing below 600°C, the magnetic properties and electrical resistivity improve significantly. The changes in magnetic and electrical properties were correlated to structural changes and studied by x-ray-diffraction analysis, vibrating-sample magnetometer measurements, and microstructural analysis.