Quasicrystals (QCs) are known to exhibit unique properties as a result of their unique quasiperiodic structure. Real quasicrystalline (QC) materials, however, may exhibit complex phase structures, and as a consequence, their properties may differ from expectations. In the present work, QC coatings of the Al–Cu–Fe, Al–Cu–Fe–Cr, and Al–Pd–Mn systems were prepared by a plasma spray process, followed by heat treatments in the range 500–800 °C. The phase structure and evolution of the coatings were evaluated, and thermal diffusivity, hardness, and friction coefficient were measured. The presence of quasicrystalline and crystalline phases and their influence on these properties is systematically considered for the first time. Broadly, the coatings exhibit the properties expected of QC materials, low thermal diffusivity, high hardness, and low coefficients of friction, but it is also shown that these properties can be sensitive to the phase structure of the coatings. This suggests that phase structure may be manipulated by heat treatment to optimize the properties of QC coatings.