Epitaxial growth of Co on GaAs (001) and its in-plane magnetic anisotropy are studied using reflection high-energy electron diffraction, a high-resolution transmission electron microscope, and the magneto-optical Kerr effect. In the initial and final stages of growth, Co exists in single-crystalline body-centered-cubic (bcc) and hexagonal-closed-packed (hcp) phases, respectively, while in the middle stage the coexistence of the bcc and hcp structures is observed. For the bcc Co thin films on GaAs (001), a fourfold in-plane magnetic anisotropy with easy axes along the< 100> directions is realized and discussed.