A magnetic nanocomposite based on graphene oxide was prepared. Fe3O4 nanoparticles were loaded on graphene oxide sheets and GO‐Fe3O4 was covered by aniline‐pyrrole copolymer to afford poly(Py‐co‐Ani)@GO‐Fe3O4. This nanocomposite was characterized by Fourier transform infrared spectroscopy, transmission electron microscopy, vibrating sample magnetometry, X‐ray diffraction, thermogravimetric analysis, and X‐ray photoelectron spectroscopy techniques, and its catalytic activity was evaluated in the multicomponent synthesis of 2′‐aminospiro[indeno[1,2‐b]quinoxaline‐11,4′‐[4'H]pyran]‐3′‐carbonitrile and 2′‐aminospiro[indeno‐2,4′‐[4'H]pyran]‐3′‐carbonitrile derivatives. This magnetically separable catalyst is heterogeneous noncorrosive, highly efficient, and reusable.