This paper reports the cell to substratum and cell to cell interactions of a diverse group of microalgae based on the Extended Derjaguin, Landau, Verwey, Overbeek (XDLVO) approach using the previously reported physico-chemical surface properties. The microalgae included 10 different species of green algae and diatoms from both freshwater and saltwater environments while the substrata included glass, indium-tin oxide (ITO), stainless steel, polycarbonate, polyethylene, and polystryrene. The results indicated that acid-base interactions were the dominating mechanism of interaction for microalgae. For green algae, if at least one of the interacting surfaces was hydrophobic, adhesion at primary minimum was predicted without any energy barrier. However, most diatom systems featured energy barriers for adhesion due to repulsive van der Waals interactions. The results reported in this study are expected to provide useful data and insight into the interaction mechanisms of microalgae cells with each other and with substrata for a number of practical applications including prevention of biofouling of photobioreactors and other man-made surfaces, promotion of biofilm formation in algal biofilm photobioreactors, and developing bioflocculation strategies for energy efficient harvesting of algal biomass. Particularly, Botryococcus braunii and Cerithiopsis fusiformis were identified as promising species for biofloccuation and biofilm formation in freshwater and saltwater aquatic systems, respectively. Finally, based on the observed trends in this study, use of hydrophilic algae and hydrophilic coatings over surfaces are recommended for minimizing biofouling in aquatic systems.