Bi2MoO6, an eye‐catching member of the Aurivillius family, has recently drawn extensive interest in visible‐light‐driven photocatalytic environmental remediation and energy conversion by right of its salient features such as fascinating layered structure, appropriate band potentials, nontoxicity, and excellent thermal and chemical inertness. Enormous endeavors have been devoted to breaking out of its inherent flaws to further improve its unsatisfactory photocatalytic activity. Herein, a general overview is given to summarize the recent advances in the surface/interface modification strategies for fabricating highly active Bi2MoO6‐based nanostructures. The means and mechanisms of surface and interface modifications are concluded and discussed in some detail, including morphology regulation, facet control, defect engineering, metal deposition, and semiconductor combination. Moreover, representative photocatalytic applications of Bi2MoO6‐based nanostructures are also dialectically introduced and categorized into two main types: environmental contaminant removal and renewable energy development. Herein, the current research status of Bi2MoO6‐based photocatalysts is highlighted, informing a broad range of researchers abreast of these significant fields, as well as casting a glance at the challenges and potential of this material.