The formation of nanoquasicrystallites in stable icosahedral Al–Cu–Fe quasicrystalline thin films by implementing an indirect heating method from a single source is discussed in this paper. The final composition of the quasicrystalline thin films is found to be Al_62.9Cu_24.6Fe_12.5 using x-ray fluorescence spectroscopy. The icosahedral nanoquasicrystallites formation is studied by glancing-angle x-ray diffraction and transmission electron microscopy. The size of the nanoquasicrystallites is estimated to be 4–20 nm. The density of nanoquasicrystallites is calculated as (1 ± 2) × 10¹² cm⁻². The improvement of the icosahedral phase formation with increasing annealing temperature is also verified by measuring the change in resistivity with temperature in the range 10–300 K. The resistivity of the best film, which is obtained by annealing the as-deposited films at 700^°C for 1 h, is calculated to be ∼2000μΩ cm at room temperature and ∼4000μΩ cm at 10 K.