Carbon foams with different surface functionality and tailored texture characteristics were prepared from mixtures containing coal tar pitch and furfural in different proportions. The obtained materials were used as a host matrix for the preparation of zinc- and cobalt-mixed ferrite nanoparticles. The texture, morphology, phase composition, and the related redox and catalytic properties of the obtained composites were characterized by low-temperature nitrogen physisorption, XRD, SEM, HRTEM, FTIR, Mössbauer spectroscopy, TPR and catalytic decomposition of methanol to syngas. The impact of the carbon support on the formation of Co- and Zn-mixed ferrites was discussed in detail using KIT-6 silica-based modifications as reference samples. The catalytic behavior of the ferrites was considered in a complex relation to their composition, morphology, location in the porous matrix and metal ions distribution in the spinel sub-lattices. The higher amount of furfural in the carbon foam precursor promoted the formation of cobalt-rich, more accessible and highly active methanol decomposition to syngas spinel particles.