A strong diameter dependence is observed in the interfacial abruptness and growth rates in Si/Si 1- x Ge x axial heterostructure nanowires grown via Au-mediated low pressure CVD using silane and germane precursors. The growth of these nanowires has similarities to that of heterostructure thin films with similar compositional interfacial broadening, which increases with and is on the order with diameter. This broadening may reveal a fundamental challenge to fabrication of abrupt heterostructures via VLS growth.