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We have fabricated single crystal-like BiFeO3 (BFO) thin films by flux-mediated epitaxy using pulsed laser deposition(PLD). The Bi–Cu–O flux composition and its thickness were optimized using composition spread, thickness gradient, and temperature gradient libraries. The optimized BFO thin films grown with this technique showed larger grain size of ∼2μm and higher dielectric constant in the range of 260–340 than those for standard PLD grown films. In addition, the leakage current density of the films was reduced by two orders of magnitude compared to that of standard PLD grown films.