Abstract Carbon nanotube (CNT) film is favored in structural health monitoring of advanced composite materials, primarily due to its commendable mechanical properties and piezoresistive properties. Nonetheless, floating catalytic chemical vapor deposition (FCCVD) is an attractive method for fabrication of CNT films, and the electrical response to strain of FCCVD‐prepared CNT films is impeded by high aspect ratio and lamellar packing structure. For this purpose, FCCVD CNT films were modified by HCl dissolving Fe impurities, nano‐SiO 2 particles doping and freeze‐drying in combination to increase the spacing between CNTs and its networks as well as their strain sensitivities. It showed that the gauge factor (GF) according to the variation of resistance (Δ R/R 0 ) of the co‐modified film (CNT‐HCl‐SiO 2 film) was up to 15.6 for the tensile strain at the bottom surface of unidirectional carbon fiber reinforced plastic (CFRP) laminates during the process of bending tests. The bending cycle experiment of the CFRP showed relatively stable changes of Δ R/R 0 with the strains for CNT‐HCl‐SiO 2 film, while that of the pristine CNT film (CNT‐HCl‐0 film) displayed unstable non‐monotonic changes and that of HCl purified CNT film (CNT‐HCl‐10 film) revealed a gradual declining tendency. Moreover, the Δ R/R 0 of CNT‐HCl‐SiO 2 film exhibited excellent sensitivity to the strains of multiple bistable‐deformations of cross‐ply CFRP laminates. Strain gauge analysis indicated that a 51% increase of Δ R/R 0 of CNT‐HCl‐SiO 2 film at the 90° layer surface corresponded to the average strain of 434 με, meanwhile a 37% increase of Δ R/R 0 of the CNT film at the 0° layer surface corresponded to the strain of averagely −173.9 με, and both exhibited super high GFs of 1175 and 2108, respectively. Based on this high sensitivity, CNT‐HCl‐SiO 2 film also had the ability to predict the release of residual stress during the demoulding process of CFRP. Highlights Even SiO 2 dispersion in CNT film, increased the pristine film thickness by 10 times GF of CNT‐HCl‐SiO 2 film increased by 68% than CNT‐HCl‐0 film and by 164% than CNT‐HCl‐10 film SiO 2 doping significantly improved the stability of the CNT film's Δ R/R 0 with temperature and strain CNT‐HCl‐SiO 2 film has the ability to monitor the deformation and residual stress of CFRP