A Cr3Al compound with a DO3 structure has previously been predicted to be nearly half metal and a promising spintronics material; however, its synthesis has not been reported. Here, a Cr3Al compound with a DO3 structure is successfully prepared in thin-film form by the magnetron sputtering method. It was found that the substrate temperature is crucial to the atomic ordering, thin-film density and lattice constant. The lattice constant varies with different substrate temperatures and is smaller than the theoretical equilibrium lattice constant. Theoretical investigations on the electronic structures and magnetic properties indicate that the Cr3Al compound with a DO3 structure is a rare material with zero-gap half-metallic characteristics under an experimental lattice constant of 5.83 Å. The experimental result is in agreement with the theoretical results in magnetization, and the Cr3Al compound synthesized in this work exhibits semi-metallic-like electrical transport characteristics and positive magnetoresistance of greater than 2% in the temperature range 2-250 K.