In low-density carbon nanotube (CNT) materials, individual nanotubes form entangled networks of bundles. The mechanical properties of such network material depend on the structural properties of the networks, although such dependencies are poorly known from both experiments and simulations. The purpose of this work is to study the effect of the structural parameters of the CNT networks on the elastic and inelastic properties of thin CNT films in coarse-grained mesoscopic simulations, when the computational samples include tens of thousands of individual CNTs. In the mesoscopic model, each CNT is represented by a chain of stretchable cylindrical segments [1]. The mesoscopic force field accounts for stretching and bending of individual CNTs [1], van der Waals interaction between them [2], and load transfer through covalent cross-links [3]. First, the model is used to generate CNT thin films with continuous networks of entangled bundles as a result of dynamic self-assembly driven by van der Waals interaction and to characterize the structural properties of the network including bundle thickness and porous size distributions. Second, the in silico generated films composed of raw and cross-linked CNTs are used to predict their mechanical properties in quasi-static in-plane stretching and compression. The simulations showed that the bundle size distribution strongly affects the mechanical properties of CNT films. The stretching of CNT films with small average bundle sizes is characterized by strong irreversible reorganization of the network structure during the deformation processes. An increase in the bundle size results in the decrease of the film modulus and strength but strongly increases the ultimate strain. The compression of the CNT films results in nearly reversible coordinated folding and wrinkling of the films. This work is supported by NSF through the award CMMI-1554589. REFERENCES [1] L.V. Zhigilei, C. Wei, D. Srivastava, Mesoscopic model for dynamic simulations of carbon nanotubes, Phys. Rev. B, 71, 165417, 2005. [2] A.N. Volkov, L.V. Zhigilei, Mesoscopic interaction potential for carbon nanotubes of arbitrary length and orientation, J. Phys. Chem. C, 114, 5513-5531, 2010. [3] K.W. Kayang, A.H. Banna, A.N. Volkov, Chirality-dependent mechanical properties of bundles and thin films composed of covalently cross-linked carbon nanotubes, Langmuir, 38, 1977–1994, 2022.