In this paper, a high-quality sputtered-GeSn layer on Ge (100) with a Sn composition up to 7% was demonstrated. The crystallinity of the GeSn layer was investigated via high-resolution X-ray diffraction (HR-XRD) and the strain relaxation degree of the GeSn layer was evaluated to be approximately 50%. A novel method was also proposed to evaluate the averaged threading dislocation densities (TDDs) in the GeSn layer, which was obtained from the rocking curve of GeSn layer along the (004) plane. The photoluminescence (PL) measurement result shows the significant optical emission (1870 nm) from the deposited high-quality GeSn layer. To verify whether our deposited GeSn can be used for optoelectronic devices, we fabricated the simple vertical p-i-n diode, and the room temperature current–voltage (I–V) characteristic was obtained. Our work paves the way for future sputtered-GeSn optimization, which is critical for optoelectronic applications.