Chromium metallacrowns have been proposed for many applications from a potential qubit, a molecular building block, a lithographic resist, to a host for different solvent molecules. The chemical variety and versatility of these molecules are what makes them a multifunctional platform. [Pr2NH2][Cr7NiF8(O2C-tBu)16] - Cr7Ni metallacrown has been identified as a potential qubit and assemblies of it have been made by functionalisation with rigid ligands and proposed as qubit gates. Moreover, even though there are plenty examples of metallacrowns binding different species to its cavity, there are no examples of metallacrowns capturing gas molecules. Firstly, the work in this thesis shows the first examples of a metallacrown, [Cr8F8(O2C-tBu)16] â Cr8, that adsorbs gases inside of its cavity. Cr8 binds CO2, SO2, HNO3âH2O, H2S, Cl2, Br2, and I2. The binding of all the tested gas molecules and underlying interactions are studied through single crystal X-ray diffraction, and thermodynamic experiments, and computational calculations for CO2, and SO2 complexes. Secondly, Cr7Ni has been functionalised with a flexible ligand that has been further used to build an assembly of an intertwined 1D coordination polymer. The assembly was probed through EPR spectroscopy. All in all, the work presented in the thesis has demonstrated the versatility of the chromium metallacrowns to be tested for different potential applications, especially for gas adsorption and for building supramolecular assemblies.