High-quality transition metal tellurides, especially for WTe2, have been demonstrated to be necessarily synthesized under close environments and high temperatures, which are restricted by the low formation Gibbs free energy, thus limiting the electrochemical reaction mechanism and application studies. Here, we report a low-temperature colloidal synthesis of few-layer WTe2nanostructures with lateral sizes around hundreds of nanometers, which could be tuned the aggregation state to obtain the nanoflowers or nanosheets by using different surfactant agents. The crystal phase and chemical composition of WTe2nanostructures were analyzed by combining the characterization of X-ray diffraction and high-resolution transmission electron microscopy imaging and elements mapping. The as-synthesized WTe2nanostructures and its hybrid catalysts were found to show an excellent HER performance with low overpotential and small Tafel slope. The carbon-based WTe2–GO and WTe2–CNT hybrid catalysts also have been synthesized by the similar strategy to study the electrochemical interface. The energy diagram and microreactor devices have been used to reveal the interface contribution to electrochemical performance, which shows the identical performance results with as-synthesized WTe2–carbon hybrid catalysts. These results summarize the interface design principle for semimetallic or metallic catalysts and also confirm the possible electrochemical applications of two-dimensional transition metal tellurides.Supplementary InformationThe online version contains supplementary material available at 10.1186/s11671-023-03796-7.