The controlled deposition of CoCrFeNiMo0.2 high-entropy alloy (HEA) microparticles was achieved by using laser-induced forward transfer (LIFT). Ultra-short laser pulses of 230 fs of 515 nm wavelength were tightly focused into ∼2.4 μm focal spots on the ∼50-nm thick plasma-sputtered films of CoCrFeNiMo0.2. The morphology of HEA microparticles can be controlled at different fluences. The HEA films were transferred onto glass substrates by magnetron sputtering in a vacuum (10−8 atm) from the thermal spray-coated substrates. The absorption coefficient of CoCrFeNiMo0.2α≈6×105 cm−1 was determined at 600-nm wavelength. The real and imaginary parts of the refractive index (n+iκ) of HEA were determined from reflectance and transmittance by using nanofilms.