Herein, nano-kaolin/Ti⁴⁺/Fe₃O₄ as a new magnetic nano-catalyst was synthesized, and its structural properties were characterized using various techniques such as Fourier transform infrared (FTIR) spectroscopy, field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), a vibrating sample magnetometer (VSM), thermogravimetric analysis (TGA) and energy-dispersive X-ray spectroscopy (EDX). This catalyst was used for the synthesis of pyrimido[2,1-b]benzothiazoles via the one-pot condensation of 2-aminobenzothiazole, an aldehyde and β-keto ester under solvent-free conditions at 100 °C. This simple protocol has many advantages such as easy workup, high product yields, short reaction times and reusability of the catalyst.