We present temporal and spectral analysis of simultaneous 0.5-79 keV Swift-XRT and Nuclear Spectroscopic Telescope Array observations of the magnetar 4U 0142+61. The pulse profile changes significantly with photon energy between 3 and 35 keV. The pulse fraction increases with energy, reaching a value of ≈20%, similar to that observed in 1E 1841-045 and much lower than the ≈80% pulse fraction observed in 1E 2259+586. We do not detect the 55 ks phase modulation reported in previous Suzaku-HXD observations. The phase-averaged spectrum of 4U 0142+61 above 20 keV is dominated by a hard power law (PL) with a photon index ΓH ~ 0.65, and the spectrum below 20 keV can be described by two blackbodies, a blackbody plus a soft PL, or by a Comptonized blackbody model. We study the full phase-resolved spectra using the e± outflow model of Beloborodov. Our results are consistent with the parameters of the active j-bundle derived from INTEGRAL data by Hascoe¨t et al. We find that a significant degeneracy appears in the inferred parameters if the footprint of the j-bundle is allowed to be a thin ring instead of a polar cap. The degeneracy is reduced when the footprint is required to be the hot spot inferred from the soft X-ray data.