Carbon nanotube (CNT) films show great promise as an advanced bulletproof materials due to their excellent energy dissipation ability under impact loadings. However, it is challenging to determine the optimized architecture structure of CNTs to enhance the impact resistance of CNT films. In this study, the impact behavior of CNT films with various architecture structures werestudied by micro-ballistic impact experiments and coarse-grained molecular dynamics (CGMD) simulations. The micro-ballistic impact experimental results showed that the cross-ply laminated (CPL) structure enhances significantly the specific energy absorption (SEA) of CNT films compared to that with disordered structure due to the synergistic interactions between covalent bonds in CNT chains. On this basis, four CPL-CNT (CCNT) films with the same areal density (ρ2D) but different single-layer areal density ( ) and one disordered CNT (DCNT) film with the same ρ2D as the CCNT films wereconstructed in CGMD models. The simulation results showed that the SEAs of all the four CCNT films are higher than DCNT film, which is consistent with experiments. In addition, the SEAs of CCNT films increase with decreasing . However, too small can lead to local plugging failure of the CNT film and therefore decrease SEA of the CNT film. Moreover, adding crosslinks could further increase the SEAs of both the DCNT and the CCNT films due to the strengthened interactions of adjacent CNTs. The crosslinked CCNT films with appropriate ρ2D is still much higher than the crosslinked DCNT films. Furthermore, it wasfurther found that when the strength of the crosslinks aligns with that of the CNT beads, the CNT film achieves preeminent impact resistance. This study provides a pathway for enhancing the impact resistance of CNT films by optimizing the microstructure and introducing crosslinks betweenCNTs.