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[Display omitted] • Facile and scalable self-assembly of perylene diimide polymer with carbon paper. • Effective facilitation of carrier separation by π-π built-in electric field. • Narrowed band gap and low VB due to the VB tail states induced by π-π interactions. • Enhanced photocatalytic water oxidation activity of the PDIP/CP photocatalyst sheet. • Suitability of the PDIP/CP photocatalyst sheet for large-scale applications. Photocatalytic water splitting is a highly promising future energy technology. In contrast to the extensive work on particulate photocatalysts, there is still a lack of sufficient investigation for regularized photocatalysts. Here, from perylene diimide polymer (PDIP) and commercial carbon paper (CP), we develop a self-assembled PDIP/CP photocatalyst sheet that is easily scalable and can be used for photocatalytic water oxidation. Driven by strong interfacial π-π interactions, the PDIP spontaneously adsorbs onto the CP, which leads to a narrowed band gap, down-shifted VB edge, and enhanced separation of the photogenerated charge carriers of the PDIP. Under visible light, the PDIP/CP photocatalyst sheet shows significantly enhanced photocatalytic water oxidation activity (4 h cumulative oxygen evolution is 1.7 times higher than that of the powder-suspended system) and considerable cycling stability. The PDIP/CP photocatalyst sheet has the potential for large-scale device applications. [ABSTRACT FROM AUTHOR]