A novel layered AgBr-based nanocomposite (designated as AgBr-NC) was prepared using nanosecond pulsed laser ablation in liquids (PLAL) in the presence of cetyltrimethylammonium bromide (CTAB). The obtained layered AgBr-NC possesses well-defined 2D shape. X-ray diffraction (XRD) pattern was composed of a series of peaks that could be indexed to (001) reflections of a layered structure, and the basal spacing of 20.0 angstroms indicated that the surfactant was included between the AgBr interlayers in an interdigitated bilayer arrangement. In this work, we provide an experimental proof for the synthesis of a novel layered two-dimensional (2D) AgBr-NC nanosheet using PLAL in the presence of CTAB. The formation mechanism of 2D nanocomposites is also discussed.