Here, we report two new multicomponent crystals (1 and 2) using 2,7-diphenyl-9H-carbazole as the static fragment and two highly mobile components: 1,4-diazabicyclo[2.2.2]octane (DABCO) and tetrahydrofuran (THF). Our findings indicate that their motion does not take place in an isotropic and multiaxial manner, as it occurs in many inclusion compounds, but rather, two independent hydrogen bonds act as specific rotational axes within the crystals. Highly symmetric DABCO rotates over an N–H···N axis, while THF preferentially rotates around a weak C–H···O axis that is perpendicular to that of DABCO. Dynamic characterization of 1 by VT 2H NMR experiments supports that DABCO experiences rapid jumps of 120° (threefold) with a krot > 10 MHz at 300 K and 5 MHz at 150 K. At the same time, THF experiences 180° jumps in the fast regime, even at 175 K. Complementarily, 1H(T1) relaxometry studies show that DABCO has an Ea = 3.5 kcal/mol, while for THF, an Ea = 2.3 kcal/mol was computed by periodic DFT. Non-isotropic mobility of two constituents within crystals is extremely rare and could have strong implications for future applications of multicomponent solids with regulated dynamics.