This review provides an overview of the precursor chemistry that has been developed around the phase‐change material germanium‐antimony‐telluride, Ge2Sb2Te5 (GST). Thin films of GST can be deposited by employing either chemical vapor deposition (CVD) or atomic layer deposition (ALD) techniques. In both cases, the success of the layer deposition crucially depends on the proper choice of suitable molecular precursors. Previously reported processes mainly relied on simple alkoxides, alkyls, amides and halides of germanium, antimony, and tellurium. More sophisticated precursor design provided a number of promising new aziridinides and guanidinates.