The present study has a dual aim of supporting magnetic nanoparticles over the nanolayers of LDHs and designing two-dimensional magnetic nano-nets of cobalt ferrite. In this trend, nanoparticles of CoFe2O4 were prepared and supported by Co-Fe LDH through urea hydrolysis. The nanolayered structures of Co-Fe LDH were confirmed by X-ray diffraction, energy-dispersive X-ray spectrometry, FT-IR spectra, thermal analyses, and transmission electron microscopy. In addition, they indicated that 13.2% CoFe2O4 were supported over Co-Fe LDH. Transformation of the nanolayered structures of Co-Fe LDH to nano-nets was achieved by the catalytic effect of the supported CoFe2O4 nanoparticles through solvent thermal technique. X-ray diffraction patterns and transmission electron microscopy images confirmed the transformation of the supported Co-Fe LDH to nano-nets of cobalt ferrite. In order to indicate the effect of the LDH for designing the nano-nets, nanoparticles of cobalt ferrite were prepared by the same technique without LDH. The magnetic behavior of the nano-nets and the supported Co-Fe LDH were measured and compared with the nanoparticles through vibrating sample magnetometer technique. The magnetic parameters indicated that the prepared nano-nets have ferromagnetic behavior and high coercivity. However, the prepared nanoparticles revealed a superparamagnetic state and low coercivity. The experimental results concluded that the incorporation of nanoparticles with nanowires into nano-net structures has been found to be an efficient way to improve their magnetic properties and prevent their agglomerations. Finally, layered double hydroxides are an important source for constructing magnetic nanolayered structures and nano-nets.