ABSTRACTIn an effort to accelerate simulations exploring deformation mechanisms in semicrystalline polymers, we have created structure‐based coarse‐grained (CG) models of polyethylene and evaluated the extent to which they can simultaneously represent its amorphous and crystalline phases. Two CG models were calibrated from target data sampled from atomistic simulations of supercooled oligomer melts that differ in how accurately they represent the distribution of bond lengths between CG sites. Both models yield semicrystalline morphology when simulations are performed at ambient conditions, and both accurately predict the glass transition and melt temperatures. A thorough evaluation of the models was then conducted to assess how well they represent various properties of the amorphous and crystalline phases. We found that the model that more faithfully reproduces the target bond length distribution poorly represents the crystalline phase, which results from its inability to reproduce correlations in the structural distributions. The second model, which utilizes a harmonic bond potential and thus reproduces the target bond length distribution less accurately, represents the structure and chain mobility within the crystalline phase more realistically. Furthermore, the latter model more faithfully reproduces the vastly different relaxation timescales of the phases, a critical feature for modeling deformation mechanisms in semicrystalline polymers. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019, 57, 331–342