Ball-in-ball CuSCN hollow architecture is successfully synthesized by a facile one-pot aqueous solution method in the presence of poly(vinylpyrrolidone) at room temperature. The as-synthesized products are characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), UV-vis diffuse reflectance absorption spectra (DRS) and nitrogen adsorption-desorption measurement. A possible formation mechanism for CuSCN hollow sph...