Abstract The search for multiferroic materials with simultaneous ferroelectric and ferromagnetic properties in a single phase at room temperature continues to be fuelled from the perspective of developing multifunctional devices. Here we design a single-phase multiferroic La 0.67 Sr 0.33 MnO 3 -BaTiO 3 film, which possesses epitaxial single-crystal and solid-solution structure, high magnetic Curie temperature (~640 K) as well as switchable ferroelectric polarization. Moreover, a notable strain-mediated magnetoelectric coupling at room temperature in the way of modulating the magnetism with an external applied voltage is also observed. The synthetic solid-solution multiferroic film may open an extraordinary avenue for exploring a series of room-temperature multiferroic materials.