Industrial emissions, environmental monitoring, and medical fields have put forward huge demands for high-performance and low power consumption sensors. Two-dimensional quasicrystal (2D QC) nanosheets of metallic multicomponent Al 70 Co 10 Fe 5 Ni 10 Cu 5 have emerged as a promising material for gas sensors due to their excellent catalytic and electronic properties. Herein, we demonstrate highly sensitive and selective NO 2 sensors developed by low-cost and scalable fabrication techniques using 2D QC nanosheets and α-Fe 2 O 3 nanoparticles. The sensitivity (ΔR/R%) of the optimal amount of 2D QC nanosheet-loaded α-Fe 2 O 3 sensor was 32%, which is significantly larger about 3.5 times than bare α-Fe 2 O 3 sensors for 1 ppm of NO 2 at 150 °C operating temperature. The sensors exhibited p-type conduction, and resistance was reduced when exposed to NO 2 , an oxidizing gas. The enhanced sensing characteristics are a result of the formation of nanoheterojunctions between 2D QC and α-Fe 2 O 3 , which improved the charge transport and provided a large sensing signal. In addition, the heterojunction sensor demonstrated excellent NO 2 selectivity over other oxidizing and reducing gases. Furthermore, density functional theory calculation examines the adsorption energy and charge transfer between NO 2 molecules on the α-Fe 2 O 3 (110) and QC/α-Fe 2 O 3 (110) heterostructure surfaces, which coincides well with the experimental results. KEYWORDS: α-Fe 2 O 3 , two-dimensional quasicrystal, heterostructures, NO 2 sensor, DFT