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The heterojunction effect can effectively improve the separation efficiency of the photocatalyst’s photo-generated electron and hole pairs, thereby greatly improving the photocatalytic hydrogen production performance of the photocatalyst. In this paper, Bi6O6(OH)3(NO3)3 · 1.5H2O (BBN) and ZnO are used to construct and synthesize Bi6O6(OH)3(NO3)3 · 1.5H2O/ZnO (BBN/ZnO) heterojunction photocatalyst. Under UV-vis light irradiation, the BBN/ZnO composite could generate H2 with a rate of 28.66 μmol·g−1·h−1, which is higher than pure BBN (0.92 μmol·g−1·h−1) and ZnO (6.54 μmol·h−1·g−1) at around 31.1 and 4.4 times, respectively. Moreover, the experimental results found that the composite still exhibits excellent photocatalytic activity and maintains a high and stable activity in the 12-hour experiment with 3 cycles. The possible mechanism to enhance the photocatalytic behavior is attributed to the expanded light absorption range, reduced surface migration resistance, and inhibited recombination of photo-generated electron and hole pairs.