Enhanced boiling heat transfer via surface engineering is a topic of general interest for its great demand in industrial fields. However, as a dynamic interfacial phenomenon, a deep understanding of its process and mechanism, including liquid re-wetting and vapor departure, is still challenging. Herein, a micro-/nanostructured Cu surface containing a periodic microgroove/pyramid array with rich nanowrinkles is designed, where superspreading (<134.1 ms) of organic cooling agents highly boosts the liquid re-wetting process, causing a discontinuous solid-liquid-vapor three-phase contact line and ultralow under-liquid bubble adhesion force (≈1.3 μN). Therefore, a characteristic, ultrafast jet-flow boiling (bubbles rapidly ejected in multiple strips) is obtained on this surface, giving a priority to nucleation (superheat ≈ 1.5 °C) and simultaneously enhancing the critical heat flux and heat-transfer coefficient by up to 80% and 608%, respectively, compared with a flat surface. In situ observation and analysis of the nucleation, growth, and departure of micro-sized jet-flow bubbles reflects that microgrooves/pyramids with nanowrinkles promote the latent heat exchange process by superspreading-induced ultrafast liquid re-wetting and constant vapor film coalescing. Based on the designed structures, high-performance phase-change cooling for central processing unit heat management in supercomputer centers is accomplished with an ultralow power usage effectiveness (PUE < 1.04).