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Abstract Strong shear thickening and jamming in dense suspensions are driven by friction as particles are sheared into contact. Control over these frictional interactions can be achieved via particle shape and roughness, and also via the particles’ surface chemistry and interactions with the surrounding solvent. We report on experiments with cornstarch suspensions where effective friction is modified by solvent-induced interactions, focusing on the effect of hydrogen bonding between solvent molecules and hydroxyl groups on the particle surface. We systematically vary the hydrogen bonding propensity by increasing the size of the backbone of the solvent molecule, from water to diols with up to 4 carbon atoms. For a fixed particle weight fraction, we find a sudden transition from strong shear thickening (in water and ethylene glycol) to shear thinning (in propanediol and butanediol). Combining data from rheology, density functional theory simulations, and fixed-rate pull tests, our results show how changes in the solvent’s molecular structure affect both particle–solvent and solvent–solvent interactions, and how this can be used to tailor the shear-thickening and jamming behavior of suspensions.