ABSTRACT While large π‐conjugated nanoribbons possess highly tunable electronic properties, their potential in high‐performance organic photovoltaics (OPVs) remains largely untapped. Herein, we report a π‐extended nanoribbon‐like electron acceptor, PDIY, featuring a molecular length of 4.85 nm (11 fused rings) and near‐infrared absorption extending to 900 nm. PDIY is engineered with a perylene diimide core fused to dual rylene units and end‐capped with Y‐type acceptor moieties. The rigid conjugated framework effectively suppresses conformational/vibronic relaxation, weakens electron‐phonon coupling, and yields an intrinsically low non‐radiative voltage loss (Δ V nr ) of 0.146 eV, among the lowest values reported to date, thereby enabling higher open‐circuit voltage. Despite its large size, the twisted geometry of PDIY leads to a unique “low crystallinity, strong aggregation” behavior. This allows PDIY to serve as a potent morphology‐directing additive that acts in a manner consistent with heterogeneous nucleation, inducing the formation of robust, large‐diameter fibrillar networks within bulk‐heterojunction blends. Consequently, the integration of PDIY yields a simultaneous enhancement across all photovoltaic parameters, boosting power conversion efficiencies (PCEs) from 19.62% to 20.57%. This work establishes twisted nanoribbon‐like acceptor as a versatile molecular platform for the dual regulation of excited‐state dynamics and active‐layer morphology in next‐generation OSCs.
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