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Inspired by gradient materials in nature, advanced engineering components with controlled structural gradients have attracted substantial research interests due to their exceptional combinations of properties. However, it remains challenging to generate structural gradients that penetrate through bulk materials, which is essential for achieving enhanced mechanical properties in metallic materials. Here, we report practical strategies to design controllable structural gradients in bulk metallic glasses (BMGs). By adjusting processing conditions, including holding time and/or controlling temperatures, of cryogenic thermal cycling and fast cooling, two different types of gradient metallic glasses (GMGs) with spatially gradient-distributed free volume contents can be synthesized. Both mechanical testing and atomistic simulations demonstrate that the spatial gradient can endow GMGs with extra plasticity. Such an enhanced …