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Carbon nanofibers (CNFs) with excellent conductivity and stability have become a promising material to design the strain sensing network. To date, however, the effect of the stacked structure of CNF membrane on the sensing performance has rarely been studied. In this work, we reported a high-performance sensor based on the cross-stacked aligned CNF membrane. The effects of cross-stacked structures on the sensing characteristics were systematically investigated. The flexible strain sensor could capture low detection limit (<0.1%) with a gauge factor (GF) of 4.24 and wide strain range up to 130%. The uniform GF value reached 2050 when the strain was in the range of 100–130%. In addition, the high linearity under 40% strain (>0.998), excellent durability and quick response time (<200 ms) were demonstrated. The excellent comprehensive performances were simultaneously obtained. The sensor could be used in extensive applications, such as monitoring body movements and distinguishing the track of writing. [ABSTRACT FROM AUTHOR]