Fundamental deformation mechanisms of FCC materials under indentation have been probed at the grain scale. Experimental tests have been conducted on large-grained annealed and cold-worked polycrystalline nickel samples with a Berkovich indenter. Indentation axes have been chosen to be close to the three main crystallographic directions [001], [101] and [111]. Pileups and slip traces have been revealed around the residual imprints by analysing topographic measurements obtained by atomic force microscopy. It is shown that the indenter orientation in each indentation plane drives pileups and slip traces which in turn contain precious information about the crystallographic orientation and the hardening state of the studied grain. Imprint topographies after pileup formation therefore carry information that one can exploit to assess some intrinsic material properties at the grain scale. A 3D finite element modelling of the nanoindentation test at the grain scale has been developed, making use of crystal plasticity constitutive laws. Six different virtual materials having the same macroscopic behaviour have been built. The simulation results show a good agreement with experimental tests and also a great pileup sensitivity to interaction matrix components. These results pave the way to the interaction matrix identification using an inverse finite element method. 1-Introduction Whether based on continuum mechanics or dislocation dynamics, crystal plasticity models involve generally a great number of material parameters, making the description of the phenomena very complete (