In the present study, the wear behaviour of two aluminium alloys (AA-5754 and AA-5083) is analysed where these have been previously processed by severe plastic deformation (SPD) with equal channel angular pressing (ECAP). In order to achieve the objectives of this study, several disks made of these alloys are manufactured by isothermal forging from different initial states. The microstructures of the initial materials analysed in this study have different accumulated deformation levels. In order to compare the properties of the nanostructured materials with those which have not been ECAP-processed, several disks with a height of 6 mm and a diameter of 35 mm are manufactured from both aluminium alloys (that is, AA-5754 and AA-5083) isothermally forged at temperatures of 150 and 200 °C, respectively. These thus-manufactured disks are tested under a load of 0.6 kN, which is equivalent to a stress mean value of 18 MPa, and at a rotational speed of 200 rpm. In order to determine the wear values, the disks are weighed at the beginning, at 10,000 revolutions, at 50,000 revolutions and at 100,000 revolutions, and then the volume-loss values are calculated. This study was carried out using specific equipment, which may be considered to have a block-on-ring configuration, developed for testing in-service wear behaviour of mechanical components. From this, the wear coefficients for the two materials at different initial states are obtained. In addition, a comparison is made between the behaviour of the previously ECAP-processed aluminium alloys and those that are non-ECAP-processed. A methodology is proposed to determine wear coefficients for the aluminium alloys under consideration, which may be used to predict the wear behaviour. It is demonstrated that AA-5754 and AA-5083 aluminium alloys improve wear behaviour after the ECAP process compared to that obtained in non-ECAP-processed materials.