Present manuscript elicits an account of the sonication promoted multicomponent reactions strategy assisted by multiwalled carbon nanotubes embraced with nickel‐ferrite (NiFe2O4‐CNTs) magnetic nanoparticles, as a heterogeneous catalyst to synthesize a novel series of pharmacologically active benzo[d]imidazo[2,1‐b]thiazole scaffolds. The synthesis of these biologically active derivatives was achieved via. A3 coupling involving 2‐aminobenzothiazole, pertinent aryl aldehydes and phenyl acetylene derivatives, proceeded in PEG 400 as green solvent under aerobic conditions to afford the products in good to excellent yields. The higher environmental compatibility and sustainability factors such as higher ecoscale score, smaller E‐factor and appreciable atom economy put this etiquette under the parasol of green chemistry precepts. The characterization of synthesized catalysts was attained through varied techniques viz. powder X‐ray diffraction, field emission scanning electron microscopy with energy‐dispersive X‐ray spectroscopy, Raman, FT‐IR, VSM and TGA‐DTA‐DTG analyses, dispersion studies, and nitrogen porosimetry analyses. The structures of the synthesized compounds were also endorsed by extensive spectroscopic studies (FT‐IR, 1H and 13C NMR, Mass) and elemental analyses.