The present work utilizes single molecule methods and analysis to investigate soft and hard substrates. First, the effect of charged hard surfaces on charged probes were evaluated, as the soft surfaces were built upon such a structure. Then, selected polymers were selected according to their importance in smart surface technology. The extent of interaction of the selected probes with the array of soft surfaces gives insight to the potential tunability of these surfaces. The three distinct polymers range from ubiquitous usage to advancements in current technology. The studies presented here are needed to characterize, on the nanoscale, the Coulombic interactions of these polymers.