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We present a self-driven long-range electrophoresis of organic nanocrystals facilitated by a rationally designed photogenerated outer electric field (OEF) on their surface. Employing perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) molecular nanocrystals as a model system, we demonstrate that a directional OEF with an intensity of 13.6-0.4 kV m-1 across a range of 25-200 μm. This OEF-driven targeted electrophoresis of PTCDA nanocrystals onto the microplastic surface enhances the activity for subsequent decomposition of microplastics (196.8 mg h-1) into CO2 by solid-solid catalysis. As supported by operando characterizations and theoretical calculations, the OEF surrounds PTCDA nanocrystals initially, directing from the electron-rich (0 1 1) to the hole-rich (1 12) surface. Upon surface charge modulation, the direction of OEF changes toward the solid substrate. The omnipresent OEF-driven electrophoretic effect in organic nanocrystals with anisotropic charge-enrichment characteristics indicates potential advancements in realizing effective solid-solid photocatalysis.