We studied in detail the in-plane magnetic properties of heterostructures based on a ferroelectric BaTiO 3 overlayer deposited on a ferromagnetic La 2/3 Sr 1/3 MnO 3 film grown epitaxially on pseudocubic (001)-oriented SrTiO 3 , (LaAlO 3 ) 0.3 (Sr 2 TaAlO 6 ) 0.7 and LaAlO 3 substrates. In this configuration, the combination of both functional perovskites constitutes an artificial multiferroic system with potential applications in spintronic devices based on the magnetoelectric effect. La 2/3 Sr 1/3 MnO 3 single layers and BaTiO 3 /La 2/3 Sr 1/3 MnO 3 bilayers using the pulsed-laser deposition technique. We analyzed the films structurally through X-ray reciprocal space maps and high-angle annular dark field microscopy, and magnetically via thermal demagnetization curves and in-plane magnetization versus applied magnetic field loops at room temperature. Our results indicate that the BaTiO 3 layer induces an additional strain in the La 2/3 Sr 1/3 MnO 3 layers close to their common interface. The presence of BaTiO 3 on the surface of tensile-strained La 2/3 Sr 1/3 MnO 3 films transforms the in-plane biaxial magnetic anisotropy present in the single layer into an in-plane uniaxial magnetic anisotropy. Our experimental evidence suggests that this change in the magnetic anisotropy only occurs in tensile-strained La 2/3 Sr 1/3 MnO 3 film and is favored by an additional strain on the La 2/3 Sr 1/3 MnO 3 layer promoted by the BaTiO 3 film. These findings reveal an additional mechanism that alters the magnetic behavior of the ferromagnetic layer, and consequently, deserves further in-depth research to determine how it can modify the magnetoelectric coupling of this hybrid multiferroic system.