An efficient and environmentally sustainable domino protocol has been presented for the synthesis of structurally diverse spiroannulated indolo[3,2‐c]quinolines involving three component sequential reaction of phenylhydrazine, o‐aminoacetophenone and cyclic ketones using nanostructured terbium doped TiO2 as recyclable and reusable heterogeneous catalyst. The nanostructured catalyst was synthesized successfully and characterized by X‐ray Diffraction (XRD), transmission electron microscopy (TEM), EDX and Fourier transform infra‐red spectroscopy (FTIR). The substitution of Ti+4 with Tb+3 and the formation of Ti‐O‐Tb bonds as a result of doping of Terbium with TiO2 NPs increases the catalytic efficiency and facilitates the reaction to provide the products in excellent yields. The present protocol with special features; operational simplicity, atom‐economy, mild reaction conditions, environmental sustainability and high synthetic efficiency with recyclability and reusability of catalyst has been reported for the first time to synthesize spiroannulated indoloquinolines and expecting to provide the library of promising new leads in drug discovery research.