Amongst colloidal gels, those designed by the assembly of anisotropic colloidal particles tend to form fibrillar gels and are attracting interest as artificial cell growth environments since they have a structure reminiscent of biological extracellular matrices. Their properties can be tuned by controlling the size, shape, and rigidity of the nanoparticles used during their formation. Herein, the relationship between the physical and mechanical properties of the nanocolloidal building blocks and the properties of the resulting gels is investigated. Thermoresponsive particles with different aspect ratios and controlled rigidity were prepared, and the gelation and the properties of the resulting gels were studied. The results show how the aspect ratio and rigidity of polymer colloids tune the properties of the gels. An increase in the aspect ratio of the nanocolloid used led to a sol–gel transition observed at lower particle concentration, but an increase in the rigidity of the nanocolloids delayed the sol–gel transition to higher concentration. However, at a constant concentration, increases in the anisotropy produced gels with higher modulus and lower yield strain. Similarly, an increase in rigidity of the colloids increased the modulus and reduced the yield strain of the resulting gels.