The Co–BaTiO3 nanocomposite films on the MgO (1 0 0) surface were grown with a thickness of about 30–100 nm by using the pulsed laser deposition (PLD) method. Co nanoparticles with the diameter of 5–18 nm were embedded uniformly in the BaTiO3 matrix. The measurements with the X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) indicate that the BaTiO3 matrix is grown in the (0 0 1) direction with respect to the MgO(1 0 0) surface. The AFM images show that the root of mean squared (RMS) roughness of Co–BaTiO3 ranges from 0.11 to 0.9 nm. The Raman scattering on the Co–BaTiO3 nano-composite films shows an enhanced intensity and a shifted wavenumber compared to the pure BaTiO3 crystal.