It is generally difficult to obtain single-phase quasicrystalline thin films due to the stringent requirement for composition and working parameter controls. In this paper, the magnetron sputtering preparation of a single-phase quasicrystalline film is described in detail. Three key issues are particularly addressed: target composition, process parameters, and subsequent heat treatment scheme. Firstly, an alloy ingot of composition Al63Cu25Fe12(at.%) is melted as the raw material for the target. Then thin film depositions were made in a magnetron sputtering system with 196 W and 1 h, subsequently annealed at 650 °C for 15 min to obtain single-phase quasicrystalline films. The dense and uniform film is well attached to the 304 stainless steel substrate, with a bonding force between film and substrate being 42.5±0.6 N. Such a high-quality film allows reliable characterizations on properties such as hardness (13.4±0.3 GPa), elastic modulus (218±6 GPa), hardness-over-modulus ratio (0.062±0.004), non-stick (water contact angle reaching 102±2°), corrosion resistance (self-corrosion potential −653.19 mV and self-corrosion current density 4.19 μA⋅cm−2 in 3.5 wt.% NaCl electrolyte), coefficient of friction (0.16, using 304 stainless steel ball), all falling close to those of bulk quasicrystals. The root mean square roughness of the quasicrystalline film was found to be 2.12 nm.