The deformational behaviour of linear high density polyethylene (HDPE) in simple shear to large strains and the mechanisms involved in this deformation were investigated. The specimens were sheared at a constant rate at room temperature. The structure and morphology of the samples of HDPE deformed to various permanent shear strains up to 6.3 were studied using wide-angle and small-angle X-ray scattering and transmission electron microscopy. The results show that the simple shear deformation of HDPE is controlled by crystallographic slip mechanisms, mostly the (100)[001] chain slip supported by the (100)[010] transverse slip and (010)[001] chain slip. The crystallographic deformation mechanisms were found to be active in the whole range of the strain history. At strains up to 3.0 the deformation by these mechanisms is supported by shear in the amorphous interlamellar layers (interlamellar sliding) which also alters the orientation of the crystalline phase. This sliding appears to be partially reversible on unloading. At moderate strains chain slip becomes unstable, which causes the localization of deformation within numerous fine shear bands. Further deformation concentrated in bands leads to the destruction of the crystalline lamellae and the transformation of the sample morphology into a microfibrillar one at a shear strain near 4.3. Further deformation, mostly by chain slip, in the crystals arranged after their fragmentation into microfibrils results in a sharp, nearly axial texture with the chain axis c tilted a few degrees away from the direction of shear.