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The evolution of the pore structure of compressed expanded vermiculite was investigated in situ under uniaxial stress up to 3200 bar using small-angle neutron and X-ray scattering. The studied samples have a lamellar texture in which the presence of oriented oblate pores was revealed by the anisotropic small-angle scattering patterns. The initial pore size distribution and the mechanical behaviour of the pellets at working pressure conditions are strongly related to the applied initial stresses used to pre-compact the vermiculite powder. Our study shows that the porous structure of the pellets was not modified under compression up to the pre-compaction pressure. Higher densification is associated with increasing anisotropy of the pore-matrix interface structure. The pore-matrix interface could be described with fractal geometry. The stress dependence of the system fractal dimension, apparent specific surface area and total porosity was determined and related to the meso-and macropore evolution under uniaxial stress.