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Biologically privileged fused pyrimidine spirocycles were synthesized via a metal‐free three‐component cascade reaction utilizing mercapto/aza lactam active methylene compounds. This rapid and efficient one‐pot operation quickly delivered seven different polycyclic and spirocyclic scaffolds such as pyranothiazolopyrimidine, benzothiazolopyranopyrimidine, pyranotriazolopyrimidine, benzoimidazolopyranopyrimidine, spiroindolinepyranothiazolopyrimidine, spirobenzothiazolopyranopyrimidineindoline, and spirobenzo‐imidazolopyranopyrimidineindoline at room temperature with excellent regio/chemoselectivity.

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