Molecule and ion enrichment, or depletion, at the ocean surface impacts transfer to marine aerosol and thus chemistry in both scenarios. Additionally, geochemical weathering, environmental contaminant capture, cloud droplet surface electric fields, and interfacial chemistry of materials provide the vast motivations for studies of interfacial ion pairing, binding, and surface prevalence and organization of molecules and ion assemblies at interfaces. This area of science continues to be controversial although there is growing but limited consensus: case in point, reaction rate enhancements in microdroplets. In this presentation, interfacial structure of liquid surfaces and the driving forces of such are presented using vibrational sum frequency generation spectroscopy (VSFG), second harmonic generation (SHG), Brewster angle microscopy (BAM), surface potential, surface tension, polarized Raman, and infrared reflection absorption spectroscopy (IRRAS). Some focus is on Fe(III), Al(III), Ca(II), Mg(II), and anions from the halide series to sulfate. Binding mechanisms and ion surface activity are not necessarily correlated in that the driving forces of electrostatics and nonspecific dispersion compete with surprising outcomes. Inherent and applied electric field data from aqueous surfaces is also explored to reveal inherent surface charge that varies significantly with surface structural assembly.