An Absorption‐Transport Reconfigurable 2D/3D/2D Architecture Enables Multispectral‐Adaptive Bifacial Perovskite Photovoltaics

ABSTRACT Tandem architectures have emerged as the prevailing strategy to overcome the fundamental trade‐off between broadband photon absorption and efficient photon‐energy utilization in photovoltaic devices. However, only the complex and implementation‐demanding multi‐terminal tandem configuration offers adaptability to diverse light sources. Here, we introduce an absorption‐transport reconfigurable architecture implemented in a bifacial single‐junction device, which harnesses the previously overlooked parasitic absorption of a 2D perovskite passivation layer to achieve spectral absorption separation between high‐energy blue‐violet and low‐energy green‐to‐near‐infrared photons. This design not only enables efficient bifacial operation with near‐omnidirectional light harvesting but also supports broadly applicable photon‐energy harvesting under both sunlight and artificial lighting. Notably, the V oc under blue‐light illumination reaches 1.67 V, exceeding the V oc ceiling of a 1.55 eV single‐junction absorber. In terms of applicability, a single device can deliver PCEs of 24.69% (AM 1.5G), 38.45% (warm‐white LED), and 37.55% (cool‐white TL84 fluorescent), alongside a record V oc of 1.081 V under weak illumination (1122 lux/346 µW cm −2 ). Owing to the robust interfacial anchoring design, the champion device retains >90% of its initial performance after 2000 h of continuous operation, thereby offering a viable pathway toward rapid, scenario‐agnostic deployment.