The behavior of colloids is governed to a great extent by their interactions with various chemicals which in turn are influenced by their surface properties including electrostatic charge. In the past, mechanisms of charge generation on simple solids, such as oxides, and salt types, such as calcite, and adsorption of simple species, such as chlorides, alkyl sulfonates, and water-soluble polyelectrolytes, on them have been explored and well understood. Microstructures of adsorbed layers have been probed using spectroscopic, electrokinetic, and scanning microprobe techniques and the proposed aggregation of surfactants and polymers at interfaces to form solloids(1) ("Surface cOLLOIDS" such as hemimicelles) has been verified. Interactions in simple systems have also received considerable attention. The challenge now lies in understanding complex real-life systems consisting of mixed multicomponent solids in media containing a variety of organic and inorganic species. The most exciting results will possibly come from studies of the colloidal behavior of dynamic natural colloids such as microbes. In this treatise some of the enigmas in real life systems and the challenges involved in understanding and utilizing them are explored. Future colloids and nanoids(2) will be designed so that the adsorbed layers, like the living entities, will respond to external perturbations and reorient/reconform themselves for optimum behavior. Based on the dynamics, one can envisage novel materials and processes that will perform a specific function in response to externally controlled perturbations. These novel systems will find applications for functional coatings and films, signal transmission devices, nanoelectronic circuits, and drug delivery and toxin extraction.