Herein, we demonstrate for the first time the fabrication of one-dimensional (1D) Bi₂MoO₆ inter-crossed nanosheet-built frameworks by using MoO₃ nanobelts as the growth templates and molybdate source. Especially, this novel Bi₂MoO₆ framework structure exhibits remarkably enhanced photocatalytic activity toward the degradation of organic dyes under visible-light irradiation, far exceeding that of conventional Bi₂MoO₆ nanoplates and nanoparticles. The photoelectrochemical study suggests that the hierarchical framework structure could facilitate the photoinduced charge separation and transfer from the inter-crossed Bi₂MoO₆ nanosheets, which may make a significant contribution to the enhanced photocatalytic activity.