Metal organic magnets have enormous potential to host a variety of electronic and magnetic phases that originate from a strong interplay between the spin, orbital and lattice degrees of freedom. We control this interplay in the quantum magnet CuF2(D2O)2pyz by using high pressure to drive the system through a structural and magnetic phase transition. Using neutron scattering, we show that the low pressure state, which hosts a two-dimensional square lattice with spin-wave excitations and a dominant exchange coupling of 0.89 meV, transforms at high pressure into a one-dimensional spin-chain hallmarked by a spinon continuum and a reduced exchange interaction of 0.43 meV. This direct microscopic observation of a magnetic dimensional crossover as a function of pressure opens up new possibilities for studying the evolution of fractionalised excitations in low dimensional quantum magnets and eventually pressure-controlled metal-insulator transitions.PACS numbers: 64.70. Tg, 75.30.Kz, 75.40.Gb, 75.30.Ds, 75.10.Pq, 75.30.Et Interacting spin systems with strong quantum fluctuations are an indispensable platform for exploring concepts in quantum many-body theory. For rigorous tests of theory it is often necessary to measure the system response due to external control parameters such as applied magnetic field and pressure (P ). Just modest changes in these variables afford precise control over the strongly fluctuating degrees of freedom [1], and provide a direct route towards exotic physics such as magnetic field-and P -driven quantum phase transitions [2][3][4]. Another way to tune a system is to modify directly the magnetic superexchange, such as by changing the chemistry [5,6], or by generating a sizeable in-situ modification of the crystal lattice. While the latter case proves difficult to achieve, it is much sought-after since it promises the direct control of magnetic dimensionality. Moreover, such an in-situ dimensionality change can be independent of the temperature, with such crossovers usually taking place as density of thermal fluctuations varies.The different topologies of one-dimensional (1D) and two-dimensional (2D) quantum spin systems are wellknown to define strongly contrasting ground states and dynamics. In 1D systems such as the half-integer spin chain, fermionic fractional excitations termed unbound spinons give a characteristic excitation continuum that disperses only along the chain direction [7]. In contrast, on the 2D magnetic square lattice, Néel-order and spin waves dispersing within the square lattice plane can be expected [8]. Exploring an in-situ transformation between 1D and 2D magnetic regimes is experimentally challenging due to lack of suitable materials, but it can be expected to provide both a deeper understanding of the adjacent states, and potentially the discovery of unusual phenomena in the vicinity of the crossover. For example, in recent work on 2D magnetic square lattice systems such as Cu(DCOO) 2 ·4D 2 O and La 2 CuO 4 , unusual features in the excitation spectra of each have bee...