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The method for preparation of polyisoprene includes conducting polymerization reaction of isoprene in a first organic solvent under the presence of rare earth catalyst I and rare earth catalyst II, to obtain polyisoprene with bimodal molecular weight distribution, wherein the polymerization reaction conditions are controlled to ensure the peak molecular weight of the high molecular weight component fraction in the polyisoprene is 1×106-2×106 and the peak molecular weight of the low molecular weight component fraction is 2×105-4×105, and the weight ratio of content of the high molecular weight component fraction to the low molecular weight component fraction is 1-25 : 1. The molecular weight distribution of the polyisoprene obtained with the method provided is bimodal distribution; therefore, the polyisoprene not only has the mechanical properties of polyisoprene with high molecular weight, but also has the processability of polyisoprene with low molecular weight.