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The rational design of smart bioinks has achieved considerable advances in recent years by means of controlled optimization of rheological properties, crosslinking processes, and incorporation of bioactive agents. This review gives an in-depth account of hydrogel-based smart bioinks, their design principles, physicochemical and biological properties, and printability aspects. Their use in brain tissue engineering and tumor microenvironment modelling is of special interest as their capability to replicate complex cellular structures, biochemical gradients and dynamic signalling plays a critical role. Additionally, latest trends such as recent developments in nanocomposite bioinks, co-culture, and AI-assisted bio fabrication are also discussed. Although significant advances have been made, vascularization issues, long-term functionality, and scalability issues continue to pose major barriers to clinical translation. 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