By using non-equilibrium molecular dynamics simulations, we demonstrated that thermal conductivity of Germanium nanowires can be reduced more than 25% at room temperature by atomistic coating. There is a critical coating thickness beyond which thermal conductivity of the coated nanowire is larger than that of the host nanowire. The diameter dependent critical coating thickness and minimum thermal conductivity are explored. Moreover, we found that interface roughness can induce further reduction of thermal conductivity in coated nanowires. From the vibrational eigen-mode analysis, it is found that coating induces localization for low frequency phonons, while interface roughness localizes the high frequency phonons. Our results provide an available approach to tune thermal conductivity of nanowires by atomic layer coating. devices [1][2][3]. In addition to the electronic and optical properties, thermal property of NWs has attracted more and more interests due to the potential thermoelectric applications in both power generation and refrigeration [4]. For instance, by etching the surface of silicon NWs, it has been experimentally demonstrated that thermal conductivity of Si NW can be reduced more than two orders of magnitude compared with bulk Silicon [5,6]. Moreover, remarkable reduction of thermal conductivity in core-shell [7][8][9][10], tubular [11,12], and surface-decorated [13] NWs has also been reported through various kinds of interface and surface engineering.Previous studies [7][8][9] on the reduction of thermal conductivity in core-shell NWs mainly focus on Si/Ge core-shell NWs, which is quite intuitive as Ge is a low thermal conductivity material compared to Si [14]. However, in experimental realizations, the NWs synthesised are Ge/Si core-shell NWs [1][2][3]. Very recently, both theoretical and experimental works have shown that thermal conductivity of Ge/Si core-shell NWs can be lower than that of pure GeNWs with the same cross section area [15,16]. The reduction is caused by the localization of the longitudinal phonon modes induced by the coherent resonance effect between the transverse and longitudinal modes [15].Thus the core-shell structure offers the unique opportunity to further reduce thermal conductivity of low thermal conductivity material even by coating with high thermal conductivity material.Despite these recent progresses about the thermal properties of core-shell NWs, many important and fundamental issues remain unsolved. For example, in our recent 4 work [15], thermal conductivity of Ge/Si core-shell NW is compared with that of pure GeNW with the same entire cross section area. However, thermal conductivity of NW is sensitive to the surface-to-volume ratio (SVR) and increases with the cross section area [17,18]. Coating another material outside the host NW increases the cross section area and thus can lead to the increase of thermal conductivity. Therefore, to study the effect of coating on thermal conductivity from the experimental point of view, one should compare thermal cond...