The growing demand for surfaces with bespoke wettability properties, including those with omniphobic and omniphilic characteristics, has prompted a surge of interest in the creation of sophisticated materials with carefully controlled surface attributes. The objective of this study is to synthesise and characterise GPOSS-PDMS-based omniphobic and omniphilic surfaces, and to investigate their properties using a range of techniques. The precursor solution was synthesised using GPOSS and PDMS, followed by photopolymerisation. The resulting surfaces were characterised using scanning electron microscopy (SEM), atomic force microscopy (AFM), and UV spectrophotometry. Furthermore, the hydrophobic properties of the material were examined within the bulk of the GPOSS-PDMS composite using atomic force microscopy (AFM) to assess the surface and subsurface morphology. The UV absorption spectra demonstrated notable alterations in the material’s structure subsequent to polymerisation, indicative of the formation of cross-linked networks. These findings indicate that GPOSS-PDMS-based surfaces can be effectively engineered for applications requiring controlled wettability. Further studies are required to investigate the long-term stability and potential practical applications of these materials in a range of environmental conditions.