The understanding of dynamic process of epitaxial microstructure forming in laser additive manufacturing is of vital importance for achieving products with single crystalline texture. Here, we perform in situ, real-time synchrotron Laue diffraction experiments to capture the microsturctural evolution of nickel-based single-crystal superalloys during rapid laser remelting process. In situ synchrotron radiation Laue diffraction characterises the crystal rotation behavior and stray grains formation process. With complementary thermo-mechanical coupled finite element simulation and molecular dynamics simulation, we identify that the crystal rotation is governed by the localized heating heterogeneity induced deformation gradient, and that the subgrains rotation caused by rapid dislocation movement and complex stress field could be the major mechanism in the generation of granular stray grains at the bottom of the melt pool.