In this work, a Al-Cu-Li alloy plate with outstanding mechanical properties was successfully prepared with electromagnetic twin-roll casting (TRC) technology. The microstructure of Al-Cu-Li alloy manufactured by conventional mold casting, TRC, and electromagnetic TRC was studied in detail. The action mechanism of electromagnetic oscillation field (EOF) in the TRC process was studied by systematic experimental characterization and numerical simulation. The results show that the EOF will enlarge the circumfluence area in the cast-rolling zone, accelerate the mass transfer and heat transfer in the molten pool, and make the solute field and flow field in the liquid cavity tend to be evenly distributed. Further, the introduction of the EOF will produce the electromagnetic body force F with the maximum strength of 14 N/m3. The F acting on the solidification front will eliminate the accumulation and deposition of Cu2+, Li+, Mg2+, Zn2+, Mn2+ at the dendrite tip and inhibit the growth of dendrites. At the same time, the F can refine the microstructure of the TRC plate, promote the formation of equiaxed crystals, improve the supersaturated solid solubility of solute elements in the a(Al) matrix, and avoid the appearance of obvious solute segregation area or the formation of excessive solute enrichment area. Therefore, the macro-segregation in TRC plate was significantly reduced, the solidification structure was dramatically refined, and the comprehensive properties of the alloy were remarkably improved.