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In this paper, the authors consider the processes that occur at the interfaces during nanowires (NWs) growth by the vapor→droplet liquid→solid mechanism (VLS), and how that leads to the faceting of the sidewall surface of the NWs. It is shown that faceting is possible only when the wetting scenario of the VLS growth of the NWs is accomplished due to the exit of the oblique closed‐packed faces to the sidewall surface of the NWs. Those oblique closed‐packed faces emerge at the crystallization front near the triple phase line. The faceting of the sidewall surface of the NWs can be controlled (i) by changing the contact angle of the catalyst droplet on the top of the NWs with the appropriate catalysts; (ii) by introducing the impurities into the gas phase, which decreases the free surface energy of the catalyst droplet; or (iii) by changing the temperature. [ABSTRACT FROM AUTHOR]