Non-noble nanomaterial-based quasicrystals (QC) are attractive structures due to their potential surface plasmon resonance (SPR) properties and ability to be easily exfoliated into two-dimensional (2D) sheets. Interaction with and sensing of organic molecules are applications where such 2D materials are a viable option due to their large surface area to volume ratio, providing abundant active sites for molecular interactions. In this work, a titanium-based multicomponent alloy (Ti 45 Zr 38 Ni 17 ) was exfoliated into a 2D quasicrystal (2D-Ti QC) from its bulk form via liquidphase exfoliation. Structural and optical experimental techniques were used to characterize the 2D-Ti QC. Its plasmonic nature was verified and demonstrated via the absorbance spectrum, light localization images, and far-field diffraction patterns. Dopamine sensing was demonstrated using the absorbance spectra of optically active 2D-Ti QC. The linear range of detection was obtained as ∼13−91 nM (200−1400 ppb). Molecular dynamics (MD) simulations of Ti QC were conducted to investigate its structural stability. The interaction between 2D-Ti QC and dopamine was investigated by using DFT simulations. In this way, the potential of 2D-Ti QC to be used as an organic molecule sensor has been experimentally and theoretically demonstrated.