Perego et al. designed a MOF architecture with two distinct ligands, coordinated to zinc clusters in order to form a pillar-and-layer 3D array of orthogonal rotors, with 4,4 ′ -bipyridine (bipy) as pillars and bicyclo[1.1.1]pentanedicarboxylate (BCP) linkers arranged in a layer. With two different fast molecular rotors thus assembled in 3D, their interactions lead to a range of different regimes of ultrafast dynamics, including large amplitude jumps, coordinative oscillations, as well as multiple gearing and antigearing rotation. In addition to this temperature control of the dynamics, adsorption of CO 2 was also shown to modulate the rotor dynamics, through a reduction in the rotational frequencies of bipy rings, and the loss of the dynamic bipy-BCP coupling. A 24 similar effect was also reported by the same group in other materials, namely two isostructural Al-based MOF with dipolar rotors: rotating linkers bearing geminal fluorine atoms. The authors found that the strong inter-rotor dipole-dipole interactions created a "concerted dance" of the rotors with a correlated mechanism in the empty framework. In contrast, adsorption of CO 2 triggered a reorientation of the ligands, reducing their collective dynamics and stimulating a dipole configuration change in the crystal.