A physically-based, rate and length-scale dependent strain gradient crystal plasticity framework was employed to simulate the polycrystalline plastic deformation at the microscopic level in a large-grained, commercially pure Ni sample. The latter was characterised in terms of the grain morphology and orientation (in the bulk) by micro-beam Laue diffraction experiments carried out on beamline B16 at Diamond Light Source. The corresponding finite element model was developed using a grain-based mesh with the specific grain orientation assignment appropriate for the sample considered. Sample stretching to 2% plastic strain was simulated, and a post-processor was developed to extract the information about the local lattice misorientation (curvature), enabling forward-prediction of the Laue diffraction patterns. The 'streaking' phenomenon of the Laue spots (anisotropic broadening of two-dimensional (2D) diffraction peaks observed on the 2D detector) was correctly captured by the simulation, as constructed by direct superposition of reflections from different integration points within the diffraction gauge volume. Good agreement was found between the images collected from experiments and simulation patterns at various positions in the sample.