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Using 2.93 fb−1 of e+e− collision data taken with the BESIII detector at a center-of-mass energy of 3.773 GeV, the observation of the D0→K1(1270)−e+νe semileptonic decay is presented. The statistical significance of the decay D0→K1(1270)−e+νe is greater than 10σ. The branching fraction of D0→K1(1270)−e+νe is measured to be (1.09±0.13+0.09−0.16±0.12)×10−3. Here, the first uncertainty is statistical, the second is systematic, and the third originates from the assumed branching fraction of K1(1270)−→K−π+π−. The fraction of longitudinal polarization in D0→K1(1270)−e+νe is determined for the first time to be 0.50±0.19stat±0.08syst.