Hydrated soft matter interfaces are ubiquitous in the world around us, under-pinning materials in both the natural and man-made world. Nature utilizes these interfaces for biological catalysis, filtration, nucleation control, and more.Similarly, in synthetic systems they are used to develop coatings for healthcare,improve water filtration, direct assembly processes, and many other applications. Looking to the future, promising materials in catalysis, biomedicine and materials templating could be made possible if we can properly leverage these interfaces and their structures. However, despite their wide scale importanceand use, these interfaces have yet to be fully understood, and the first step to-wards that understanding is visualization.Towards those ends, in this work both biogenic and synthetic hydrated soft matter interfacial systems are explored. On the biogenic side coccolithophores, a species of single celled marine algae, mineralize amazing calcitic shell architectures (coccoliths) using surprisingly complicated machinery. Part of this process is the accumulation of coacervate particles (complexes of metal ions and polymers) on a coccolithophore baseplate, a fibrous, anisotropic surface on which these shells are created. This work uses established in-situ fluid cell AFM techniques to explore the kinetics and assembly of coacervate attachment to this baseplate – solution interface in the early stages of the coccolith pathway. Tracking this process gives insights into the rates of coacervate attachment and self-limiting growth that could have implications for the coccolith and other biogenic crystallization pathways. This could also help unravel the complicated intermolecular interactions that govern generalized coacervate surface templating.On the synthetic side, highly tunable, amphiphilic block copolymer (BCP)thin films are used to explore how local nanoscale chemistry and topography affect hydrated film and interfacial water structure. First, in situ fluid cell AFM amplitude imaging and force spectroscopy is used to probe these local film-water structures and response to external stimuli. From this we can further learn about how these materials exist and change in aqueous solutions. Next,the BCP-water interfacial structure is investigated and through visualization of this structure, the local energetic landscape might be predicted. To probe these nanometer water-polymer interfaces on mesoscale ordered BCP thin films we use emergent 3D-AFM force mapping techniques to visualize interfacial hydrophilic and hydrophobic regions on representative volumes of interest of the films. These can be visualized not only as an appropriate section of the film surface but to tens of nanometers into solution, giving ordering and distribution of interfacial water at and near the interface. Towards predictive solution nucleation control, we also use force maps to visualize how these regions are polarized, destroyed, or emphasized upon film functionalization with positive and negative click chemistries, heating, salt incorporation, and mixed effects.Overall, using established and emergent fluid cell AFM techniques, this work examines biogenic and synthetic water-polymer interfaces and interfacial structures. This work tracks coacervate attachment and growth on biomaterial templates, probes film evolution in aqueous solutions, and visualizes spatially correlated tiers of hydrophilic and hydrophobic ordering on and above amphiphilic BCP thin films. This helps lay the groundwork towards predictive hydrated soft matter interfacial structure understanding and control.