The invention discloses multi-principle-element alloy and a method thereof for processing the surface of aluminum alloy. The alloy is prepared from, by molfraction, 14-22 parts of Co, 14-22 parts of Cr, 1-3 parts of Al, 14-22 parts of Si, 14-22 parts of Fe, 1-10 parts of Ti, 14-22 parts of Mn, 1-3 parts of B and 1-3 parts of La. The method includes the steps that an aluminum alloy substrate is firstly cleaned and subjected to sand blasting, multi-principle-element alloy powder is sprayed on the surface of the aluminum alloy substrate through a plasma spraying device, finally the plasma sprayed surface is remelted through a CO2 laser device, and then the multi-principle-element alloy is prepared. The characteristics of the high- entropy effect, the slow diffusion effect, nano phase strengthening, super-high lattice distortion and the 'cocktail effect' of the multi-principle-element alloy are utilized for a multi-principle-element alloy coating, high tenacity of the alloy can be easily kept, and the prepared coating has the beneficial effects of being high in strength, resistant to abrasion and the like.