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Fe3Al–Al2O3 double-layer coatings (DC), Fe3Al-Fe3Al/50%Al2O3–Al2O3 triple-layer coatings (TC) and Fe3Al-Al2O3 graded coatings (GC) were produced from a series of Fe3Al/Al2O3 composite powders with different compositions on low carbon steel substrate using PLAXAIR plasma spraying equipment. Friction behaviors and wear resistance of the three kinds of coatings have been investigated under different loads. Tests were carried out using an MRH-3 standard machine, in lineal contact sliding under dry condition against hardmetal, at a sliding velocity of about 1.57 ms−1. Wear rates under different loads were measured and the friction coefficients were recorded. SEM analysis was carried out to identify the wear mechanisms. The results show that the GC has higher wear-resistance than DC and TC. The tribological characteristics of graded coating were different along the depth of the coatings, and the surface of coatings with pure Al2O3 does not show the best wear resistance. The wear rate and friction coefficients were also different under different loads. The failure types of plasma-sprayed Fe3Al-Al2O3 graded coatings in lineal contact were: loosening of ceramic particles, crack nucleation and propagation, brittle fracture, plastic deformation, and adhesive wear.