Coulomb interactions were truncated at 12 Å by employing the damped shifted force method from Fennell and Gezelter. The MOF-FF parameterization methodology was carefully validated by reproducing the NTE behavior of MOF-5 and HKUST-1, featuring the same inorganic structural building units as the investigated mesoporous MOFs. The framework response to temperature was simulated by N, P, T molecular dynamics employing a Nosé-Hoover chain thermostat and Martyna-Tuckerman-Tobias-Klein (MTTK) barostat. These temperature and pressure controls have been previously assessed for use in describing flexible MOF systems. Systems were heated from 40 to 400 K in 20 K intervals. The timestep for the simulations was 1 fs and the thermostat and barostat dampening parameters were 100 fs and 2000 fs, respectively. Each temperature included an equilibration period of 0.5 ns followed by a production period of 1.0 ns, where the average volume and dynamics were investigated. The complete mechanical properties were calculated from the trajectories by analysis of the fluctuations of unit cell vectors. The Hessians H of the optimized structures as 2 × 2 × 2 supercells were calculated with a double-sided finite difference scheme based on the analytical forces using a distortion of 0.001 Å. Based on these Hessians, phonon calculations were conducted using the phonopy software package. The largest ligand was extracted from each MOF and the same force field parameters were assigned to the molecule as for the entire MOF structure. Molecular dynamics were conducted in the N,V, T ensemble, and the dynamics of the oxygen atoms of the ligand were constrained in one plane. Trajectory periods and the thermostat were identical to that of the framework simulations. The average radius of gyration of the oxygen atoms was calculated to provide a representative value of the planar size of the ligands.