Solid-acid catalysts functionalized with catalytic groups have attracted intense interest for converting cellulose into soluble products. However, design of solid-7 acid catalysts has been guided by molecular level interactions and the actual mechanism of cellulose-solid-acid catalyst particles adsorption remains unknown. Here, colloidal stability theory, DLVO, is used to rationalize the design of solid acids for targeted cellulose adsorption. In nearly all cases, an energy barrier, arising from electrostatic repulsion and much larger than the energy associated with thermal fluctuations, prevents close contact between the solid acid and cellulose. Polymer-based solid-acid substrates such as polystyrene and Nafion are especially ineffective as their interaction with cellulose is dominated by the repulsive electrostatic force. Carbon and metal oxides have potential to be effective for cellulose-solid-acid interaction as their attractive van der Waals interaction can offset the repulsive electrostatic interaction. The effects of reactor temperature and shear force were evaluated, with the finding that reactor temperature can minimize the catalyst-cellulose interaction barrier, promoting coagulation, but that the shear force in a typical laboratory reactor cannot. We have evaluated strategies for enhancing cellulose-catalyst interaction and conclude that raising reaction temperature or synthesizing acid/base bifunctional catalysts can effectively diminish electrostatic repulsion and promote cellulose-catalyst coagulation. The analysis presented here establishes a rational method for designing solid acid catalysts for cellulose hydrolysis.