The crystallization mechanisms of Si/CuSi bilayer and its recording characteristics for write-once blu-ray disc (BD-R) were investigated. It was found that Cu3Si phase appeared during the room temperature sputtered deposition. Then, the Si atoms in CuSi layer segregated and crystallized to cubic Si in Cu3Si nucleation sites as the film was annealed at 270 °C. After heating to 500 °C, the grains size of cubic Si phase grew and the hexagonal Si phase was observed. The dynamic tests show that the Si/CuSi bilayer has great feasibility for 1-4× BD-R with the bottom jitter values below 6.5%.