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Complex oxides with tunable structures have many fascinating properties,though high-quality complex oxide epitaxy with precisely controlled composition is still out of reach.Here we have successfully developed solution-based single-crystalline epitaxy for multiferroic (1-x)BiTi(1-y)/2FeyMg(1-y)/2O3-(x)CaTiO3 (BTFM-CTO) solid solution in large area,confirming its ferroelectricity at the atomic scale with strong spontaneous polarization.Careful compositional tuning leads to a bulk magnetization of 0.07 + 0.035 μB/Fe at room temperature,enabling magnetically induced polarization switching exhibiting a large magnetoelectric coefficient of 2.7-3.0 × 10-v s/m.This work demonstrates the great potential of solution processing in large-scale complex oxide epitaxy and establishes novel room-temperature magnetoelectric coupling in epitaxial BTFM-CTO film,making it possible to explore a much wider space of composition,phase,and structure that can be easily scaled up for industrial applications.