Co-substituted U-type hexagonal ferrite bulks, with composition of Ba4Ni2−xCoxFe36O60 (x=0.2, 0.4, 0.6, 0.8), were prepared by a conventional ceramic method. Saturation magnetization (4πMs), coercivity (Hc), and Curie temperature (Tc) were investigated. Anisotropy constant (K1) was calculated by fitting the magnetization curve (M-H) according to the law of approach to saturation, and anisotropy field (Ha) was calculated accordingly. The results reveal that all the samples possess the U-type hexagonal crystallographic structure. With increasing cobalt substitution content (x), the lattice parameters (a and c) almost remain the same owing to the similar radii of Ni2+ (0.72 Å) Co2+ (0.74 Å) ions. 4πMs goes up, while Hc Hc shows an opposite trend. K1 and Ha monotonously decrease resulting from that cobalt substitution weakens the c-axis orientation. Additionally, Tc increases from 467 °C to 484 °C.