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We report on the synthesis of PbTiO3–CoFe2O4 multiferroic nanocomposites and continuous tuning of their ferroelectric and magnetic properties as a function of the average composition on thin-film composition spreads. The highest dielectric constant and nonlinear dielectric signal was observed at (PbTiO3)85–(CoFe2O4)15, where robust magnetism was also observed. Transmission electron microscopy revealed a pancake-shaped epitaxial nanostructure of PbTiO3 on the order of 30 nm embedded in the matrix of CoFe2O4 at this composition. Composition dependent ferroics properties observed here indicate that there is considerable interdiffusion of cations into each other.