We investigated the gelation of cellulose nanocrystals (CNCs) in polyelectrolyte and neutral polymer solutions. Cellulose nanocrystals (CNCs) with half-ester sulfate groups produced by acid hydrolysis of wood pulp were used in this study. The microstructure of CNCs/polymer suspensions was investigated in semidilute concentration regimes by selecting carboxymethyl cellulose (CMC700) as an anionic polymer and poly(ethylene oxide) (PEO600) as a neutral polymer solution. Together with quartz crystal microbalance with dissipation monitoring (QCM-D), theology, scanning electron microscopy (SEM), and cryotransmission electron microscopy (cryo-TEM), we characterized CNCs-polymer interactions, the suspension microstructure, and the macroscopic gel flow. Significant viscosity increases at low shear rates coupled with high shear-thinning behaviors were observed in CNC colloid-CMC700 polymer mixtures, but not those CNCs in PEO600 solutions. The apparent differences between CNCs-CMC700 and CNCs-PEO600 mixtures were due to their chain confirmations. On the basis of the evaluations from STEM, cryo-TEM, and polarized optical microscopy, we proposed that the excess CMC700 molecules in solutions result in the depletion of CNCs and the formation of anisotropic domains.