Development of a novel in situ method for simultaneous growth of single crystals and thin films of a smart material spinel is achieved. Material to be grown as metal-incorporated single crystal and thin film was taken as a precursor and put into a bath containing acid as a reaction speed-up reagent (catalyst) as well as a solvent with a metal foil as cation scavenger. By this novel method, zinc aluminate crystals having hexagonal facets and thin films having single crystalline orientation were prepared from a single optimized bath. Properties of both crystals and thin films were studied using an x-ray diffractometer and EDAX. ZnAlO is a well-known wide bandgap compound semiconductor (E = 3.8 eV), ceramic, opto-mechanical and anti-thermal coating in aerospace vehicles. Thus a space_ gmr technique was found to be a new low cost and advantageous method for in situ and simultaneous growth of single crystals and thin films of a smart material.