Magnetic Nd-(Fe, Co)-B powders prepared by a modified Pechini-type chemical method are investigated. The effect of 0–100 at.% Co concentration on magnetic properties is shown. The structure and morphology of the powders are studied by electron microscopy. The average particle size is determined by electron microscopy. The internal structure of the nanoparticle agglomerates was explored by transmission electron microscopy. The Nd2Fe14B phase was determined by spot electron diffraction. The dependence of saturation magnetization and coercive force of NdFe1–xCoxB powders on the cobalt content is investigated and discussed. An increasing coercive force is observed as a result of the increase in Co content. It is shown that the absence of phase purity leads to a decrease in the coercive force in comparison with the Nd-based hard magnetic obtained by metallurgical methods.