How to facilitate photogenerated-carrier separation is an important step in developing excellent semiconductor photocatalysts for environmental pollutant removal. Herein, Ag 2 MoO 4 (AMO) nanoparticles were assembled onto the surface of BiOBr (BOB) nanosheets to construct a highly efficient Z-scheme AMO/BOB heterojunction photocatalyst. Several analytical techniques were used to elucidate the characteristics and photocatalytic mechanism of the AMO/BOB heterojunction. Photodegradation experiments for removing methylene blue under simulated-sunlight irradiation reveal that a 20%AMO/BOB heterojunction exhibits excellent photodegradation activity with η (30 min) = 93.8% and k app = 0.08638 min -1 , which were greater by 4.5 and 5.6 times in comparison with that of pure BOB and AMO, respectively. Based on the experimental and density functional theory (DFT) calculation results, it is proposed that the Z-scheme carrier transfer/separation mechanism dominates the enhanced photodegradation performance of the composite photocatalysts. Additionally, the potential application of AMO/BOB photocatalysts in degrading various organic pollutants (including organic dyes, antibiotics and other serious organic pollutants) was also investigated.