We measured the infrared vibrational properties of two copper-containing coordination polymers, [Cu(pyz)2(2-HOpy)2](PF6)2 and [Cu(pyz)1.5(4-HOpy)2](ClO4)2, under different external stimuli in order to explore the microscopic aspects of spin-lattice coupling. While the temperature and pressure control hydrogen bonding, an applied field drives these materials from the antiferromagnetic → fully saturated state. Analysis of the pyrazine (pyz)-related vibrational modes across the magnetic quantum-phase transition provides a superb local probe of magnetoelastic coupling because the pyz ligand functions as the primary exchange pathway and is present in both systems. Strikingly, the PF6- compound employs several pyz-related distortions in support of the magnetically driven transition, whereas the ClO4- system requires only a single out-of-plane pyz bending mode. Bringing these findings together with magnetoinfrared spectra from other copper complexes reveals spin-lattice coupling across the magnetic quantum-phase transition as a function of the structural and magnetic dimensionality. Coupling is maximized in [Cu(pyz)1.5(4-HOpy)2](ClO4)2 because of its ladderlike character. Although spin-lattice interactions can also be explored under compression, differences in the local structure and dimensionality drive these materials to unique high-pressure phases. Symmetry analysis suggests that the high-pressure phase of the ClO4- compound may be ferroelectric.