Microalgal biofilm, a stable community of many algal cells attached to a solid substrate, plays a significant role in the efficient accumulation of renewable energy feedstocks, wastewater treatment, and carbon reduction. The adhesion tendency of microalgal cells on solid substrates is the basis for controlling the formation and development of microalgal biofilm. To promote the adhesion of microalgal cells on solid substrates, it is necessary to clarify which surface properties have to be changed in the most critical factors affecting the adhesion. However, there have been few systematic discussions on what surface properties influence the adhesion tendency of algal cells on solid substrates. In this study, the essential principle of microalgal cell adhesion onto solid substrates was explored from the perspective of the interaction energy between microalgal cells and solid substrates. The influence of surface properties between microalgal cells and solid substrates on interaction energies was discussed via extended Derjaguin-Landau-Verwey-Overbeek (eDLVO) theory and a sensitivity analysis. The results showed that surface properties, including surface potential (ξ) and surface free energy components, significantly affect the adhesion tendency of microalgal cells on different solid substrates. When the solid surface possesses positive charges (ξ > 0), reducing ξ or the electron donor components of the solid substrate (γs-) is an effective measure to promote microalgal cell adhesion onto the solid substrate. When the solid surface possesses negative charges (ξ < 0), an increase in either γs- or the absolute value of ξ should be avoided in the process of microalgae adhesion. Overall, this research provides a direction for the selection of solid substrates and a direction for surface modification to facilitate the adhesion tendency of microalgal cells on solid substrates under different scenarios.