The mechanism inducing the breathing in flexible metal-organic frameworks, such as MIL-53(Al), is still not fully understood. Herein, the influence of lattice vibrations on the breathing transition in MIL-53(Al) is investigated to gain insight in this phenomenon. Through solid-state density-functional theory calculations, the volume-dependent IR spectrum is computed together with the volume-frequency relations of all vibrational modes. Furthermore, important thermodynamic properties such as the Helmholtz free energy, the specific heat capacity, the bulk modulus, and the volumetric thermal expansion coefficient are derived via these volume-frequency relations using the quasi-harmonic approximation. The simulations expose a general volume-dependency of the vibrations with wavenumbers above 300 cm−1 due to their localized nature. In contrast, a diverse set of volume-frequency relations are observed for vibrations in the terahertz region (< 300 cm−1) containing the vibrations exhibiting collective behavior. Some terahertz vibrations display large frequency differences over the computed volume range, induced by either repulsion or strain effects, potentially triggering the phase transformation. Finally, the impact of the lattice vibrations on the thermodynamic properties is investigated. This reveals that the closed pore to large pore phase transformation in MIL-53(Al) is mainly facilitated by terahertz vibrations inducing rotations of the organic linker, while the large pore to closed pore phase transformation relies on two framework-specific soft modes.