Two types of PHEMA-based particles, exhibiting either carboxyl or tertiary ammine functional groups, were incorporated to fibrin-agarose (FA) hydrogels, and the effect of the addition of these synthetic particles on the viscoelastic and microstructural properties of the biomaterials was evaluated. Experimental results indicated that the incorporation of both types of polymeric particles to FA scaffolds was able to improve the biomechanical properties of the biomaterials under steady state and oscillatory shear stresses, resulting in scaffolds characterized by higher values of the storage, loss, and shear moduli. In addition, the microstructural evaluation of the scaffolds showed that the nanoparticles exhibiting carboxyl functional groups were homogeneously distributed across the fibrous network of the hydrogels. The addition of both types of artificial polymeric particles was able to enhance the viscoelastic properties of the FA hydrogels, allowing the biomaterials to reach levels of mechanical consistency under shear stresses in the same range of some human native soft tissues, which could allow these biomaterials to be used as scaffolds for new tissue engineering applications.