Stannyl-substituted [(RZn)4(OR′)4] cubanes with different tin-containing alkoxy groups [Ph3SnOZnMe] (1), [Ph3SnOZnEt] (2), [Me3SnOZntBu] (3), and [Ph3SnOZntBu] (4) are easily accessible by Brønsted acid–base reaction of the corresponding triorganotin hydroxides with ZnMe2, ZnEt2, and Zn(tBu)2, respectively. All new compounds 1–4 were characterized by various spectroscopic methods and the structures of 1 and 3 were confirmed by single-crystal X-ray diffraction analysis. The thermal degradation of the precursors 1–4 under dry synthetic air (20 % O2, 80 %N2) was studied and the final oxide materials were characterized by employing powder X-ray diffraction (PXRD) analysis, inductively coupled plasma-optical emission spectrometry (ICP-OES), transmission and scanning electron microscopy (SEM and TEM), energy dispersive X-ray spectroscopy (EDX), and atomic force microscopy (AFM). Remarkably, compounds 1 and 2 proved to be suitable as single-source precursors (SSPs) for the efficient preparation of tin-doped ZnO nanoparticles with tunable tin concentrations as a promising system for steering and improving the optoelectronic properties of tin-doped ZnO. Using 3 as SSP furnishes tin-containing ZnO materials with good electron mobilities at relatively low processing temperatures (350 °C) for thin-film transistor (TFT) applications. All the thin films of tin-doped ZnO prepared by spin-coating on silicon wafers are of great homogeneity and amorphous structure, which is promising for future applications in the field of transparent conducting oxides (TCOs).