Using Molecular Dynamics simulations, we probe the effect of various pendant polar groups on the dielectric loss of polyethylene copolymers. The dielectric loss was computed using the autocorrelation function of the total dipole moment of a completely relaxed PE-X sample. Since this calculation is computationally expensive (wall time ≥ 4200 h), we explore the use of the time-temperature superposition (tTS) principle to make it more tractable. An important point is that short time MD simulations do not allow the dipole autocorrelation function to decay completely to zero. However, we find that the tTS method performed well in determining dielectric losses in the system as long as these unrelaxed components are not included in the calculation. This methodology, which provides us with a significantly faster and reliable pathway for calculation of dielectric loss, allows us to identify the role of polar side groups on the behavior of nonpolar polymeric dielectrics.