To improve the comprehensive surface performance of 6061 aluminum alloys and reduce the influence of Al dilution behavior on the coating quality, FeCoCrNi-M (M = Mn, Cu, Ti, −) high-entropy alloy coatings were prepared by a double-layer laser cladding method. The FeCoCrNi, FeCoCrNiMn and FeCoCrNiCu coatings all consisted of a single face-centered cubic (FCC) phase. The FeCoCrNiTi coating consisted of FCC, body-centered cubic (BCC), Laves and AB-type phases. The addition of Mn or Cu decreased the hardness of the FeCoCrNi coating from 209 HV to 188 or 165 HV, and increased the wear rate from 1.16 × 10−4 mm3/N·m to 1.62 × 10−4 or 3.01 × 10−4 mm3/N·m. The addition of Ti increased the hardness to 908 HV and decreased the wear rate to 2.32 × 10−5 mm3/N·m. The current density of the FeCoCrNi coating (6.37 × 10−8 A/cm2) in 3.5 wt% NaCl solution increased with Cu or Mn addition (2.15 × 10−7 or 3.26 × 10−7 A/cm2), but decreased with Ti addition (1.15 × 10−8 A/cm2). FeCoCrNi-M coatings significantly enhanced the hardness, corrosion resistance and wear resistance of the aluminum alloy substrate.