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Phytoremediation has emerged as an ecofriendly technique to reduce hazardous particulate matter (PM) in the air. Although previous studies have conducted statistical analyses to reveal PM removal capabilities of various plant species according to their leaf characteristics, the underlying physical mechanism of PM adsorption of plants remains unclear. Conventional methodologies for measuring PM accumulation usually require long-term field tests and provide limited understanding on PM removal effects of individual leaf traits of various plants. In this study, we propose a novel methodology which can compare the electrostatic interactions between PMs and plant leaves according to their trichome structures by using digital in-line holographic microscopy (DIHM). Surface characteristics of Perilla frutescens and Capsicum annuum leaves are measured to examine electrostatic effects according to the morphological features of trichomes. 3D settling motions of PMs near the microstructures of trichomes of the two plant species are compared in detail. To validate the PM removal effect of the hairy microstructures, a polydimethylsiloxane (PDMS) replica model of a P. frutescens leaf is fabricated to demonstrate accelerated settling velocities of PMs near trichome-like microstructures. The size and electric charge distributions of PMs with irregular shapes are analyzed using DIHM. Numerical simulation of the PM deposition near a trichome-like structure is conducted to verify the empirical results. As a result, the settling velocities of PMs on P. frutescens leaves and a PDMS replica sample are 12.11 ± 1.88% and 34.06 ± 4.19% faster than those on C. annuum leaves and a flat PDMS sample, respectively. These findings indicate that the curved microstructures of hairy trichomes of plant leaves increase the ability to capture PMs by enhancing the electric field intensity just near trichomes. Compared with conventional methods, the proposed methodology can quantitatively evaluate the settling velocity of PMs on various plant leaves according to the morphological structure and density of trichomes within a short period of time. The present research findings would be widely utilized in the selection of suitable air-purifying plants for sustainable removal of harmful air pollutants in urban and indoor environments. [Display omitted] • The physical mechanism of PM adsorption process of plant leaves is investigated. • Hairy microstructures on leaves increase electric field intensity near trichomes. • Electrostatic interactions between PMs and hairy plant leaves are demonstrated. • 3D settling motion of PMs near hairy trichomes on leaves is quantitatively measured. • Settling velocity of PMs is elevated near the hairy trichomes on leaves. [ABSTRACT FROM AUTHOR]