A facile, adjustable, and expandable synthetic technique to make threedimensional (3D)-nanoframework nanomaterials with super-large surface areas is of great significance in the field of electrocatalysts. In this study, spray-drying combined with thermal decomposition reduction technique is employed to synthesize singlemetal Pt, Pt-based multimetallic, and high-entropy alloy (HEA) 3D-nanoframeworks under mild conditions (at 300 °C in a H 2 atmosphere). It is found that the assynthesized Pt 3D-nanoframework shows super-large surface areas of 94.9 m 2 /g and improves electrocatalytic performance for the hydrogen evolution reaction and methanol oxidation reaction. Moreover, the addition of the Pt element could decrease the reduction temperature of other metals (Ni, Fe, Co, Cu, Ru, etc.) via the autocatalytic behavior, and thus the Pt-based multimetallic (such as PtNi, PtCo, and PtFe) and PtCoNiCuRu HEA 3D-nanoframeworks are first designed and successfully prepared with a single-phase solid solution under low thermal decomposition temperatures (300 °C) in a H 2 atmosphere.