Separators in supercapacitors (SCs) frequently suffer from high resistance and the risk of short circuits due to inadequate electrolyte wettability, depressed mechanical properties, and insufficient thermal stability. Here, we develop a high-performance regenerated cellulose separator with nano-cracked structures for SCs via a binary solvent of superbase-derived ionic liquid and dimethylsulfoxide (DMSO). The unique nano-cracks with an average width of 7.45 nm arise from the acceleration of cellulose molecular reassembly by DMSO-regulated hydrogen bonding, which endows the separator with high porosity (70.2%) and excellent electrolyte retention (329%). The outstanding thermal stability (273 °C) and mechanical strength (70 MPa) enable the separator to maintain its structural integrity under high temperatures and external forces. With these benefits, the SC utilizing the cellulose separator enables a high specific capacitance of 93.6 F g−1 at 1.0 A g−1 and a remarkable capacitance retention of 99.5% after 10,000 cycles compared with the commercial NKK-MPF30AC and NKK-TF4030. The robust and high-wettability cellulose separator holds promise as a superior alternative to commercial separators for advanced SCs with enhanced performance and improved safety.