Nanoengineered hydrogels offer the potential to design shear-thinning bioinks for three-dimensional (3D) bioprinting. Here, we have synthesized colloidal bioinks composed of disk-shaped two-dimensional (2D) nanosilicates (Laponite) and poly(ethylene glycol) (PEG). The addition of Laponite reinforces the PEG network and increases viscosity, storage modulus, and network stability. PEG-Laponite hydrogels display shear-thinning and self-recovery characteristics due to rapid internal phase rearrangement. As a result, a range of complex patterns can be printed using PEG-Laponite bioinks. The 3D bioprinted structure has similar mechanical properties compared to the as-casted structure. In addition, encapsulated cells within the PEG-Laponite bioink show high viability after bioprinting. Overall, this study introduces a new class of PEG-Laponite colloidal inks for bioprinting and cell delivery.