Multivalent glycosylated polymers and particles display enhanced binding affinity toward lectins compared to individual glycans. The design of glycopolymers with selectivity toward pathogen-associated lectins (toxins) for sensing or in antiadhesion therapy is complicated due to lectins having promiscuous binding profiles and can be considered to be pattern recognition "readers," with the capability to bind to several different glycans. Here, heterogeneous glycopolymers bearing variable densities of two different monosaccharides are synthesized by a three-step postpolymerization modification approach, enabling systematic control over composition. It is found that heterogeneous polymers displayed increased inhibitory activity, compared to homogeneous polymers, against a RCA(120) and the cholera toxin. This demonstrates that embracing heterogeneity in glycomaterials could result in improved performance or emergent properties. (c) 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 40-47