Amorphous films having a component of the stoichiometric GeTe‐Sb2Te3pseudobinary alloy system, GeSb2Te4or Ge2Sb2Te5representatively, were found to have featuring characteristics for optical memory material presenting a large optical change and enabling high‐speed one‐beam data rewriting. The material films being sandwiched by heat‐conductive ZnS layers can be crystallized (low power) or reamorphized (high power) by laser irradiation of very short duration, less than 50 ns. The cooling speed of the sandwiched film is extremely high: more than 1010deg/s, which permits the molten material to convert to the amorphous state spontaneously; whereas, a low‐power pulse irradiation of the same duration changed the exposed portion into the crystalline state. The optical constant changes between the amorphous state and the crystalline state of them were measured to be large: from 4.7+i1.3 to 6.9+i2.6 and from 5.0+i1.3 to 6.5+i3.5, respectively. The crystallized portion was known to have a GeTe‐like fcc structure by an analytical experiment using transmission electron microscopy, differential scanning calorimetry, and x‐ray and electron diffraction methods. The high crystallization speed is ascribed to (1) the pseudobinary system which can form crystalline compositions without any phase separation, (2) the high symmetry of the fcc structure which is the nearest to the random amorphous structure, (3) the high‐energy difference between the amorphous state and the fcc crystal state.