Aramid nanofibers (ANFs) have great potential for civil and military applications due to their remarkable mechanical modulus, excellent chemical reliability, and superior thermostability. Unfortunately, the weak combination of neighboring ANFs limits the mechanical properties of ANF-based materials owing to their inherent rigidity and chemical inertness. Herein, high-performance nanopapers are fabricated by introducing a tiny amount of cellulose nanofibrils (CNFs) to serve as reinforcing blocks via vacuum filtration. As a result of the formation of nanosized building blocks and hydrogen-bonding interaction of CNFs, the resultant ANF/CNF nanopaper yields a record-high tensile strength (406.43 ± 16.93 MPa) and toughness (86.13 ± 5.22 MJ m −3 ), which are 1.8 and 4.3 times higher than those of the pure ANF nanopaper, respectively. When normalized by weight, the specific tensile strength of the nanopaper is as high as 307.90 MPa•g −1 •cm 3 , which is even significantly superior to that of titanium alloys (257 MPa•g −1 •cm 3 ). The ANF/CNF nanopaper also possesses excellent dielectric strength (53.42 kV mm −1 ), superior UV-shielding performance (≥99.999% absorption for ultraviolet radiation), and a favorable thermostability (T onset = 530 °C). This study proposes a new design strategy for developing ultrathin ANF-based nanopapers combined with high reliability and thermostability for application in highend electrical insulation fields, such as 5G communication, wearable electronics, and artificial intelligence.