As a promising two-dimensional (2D) material, black phosphorus (BP) has gained great attention because of its intrinsic physicochemical characteristics. However, BP is easy to be oxidized and form various surface defects, which decreases the charge transport and makes luminescence difficult. Herein, we report a facile strategy to synthesize chemically anchored BP/chromophore composite luminescent materials by integrating 2D BP nanosheets with boron dipyrromethene (BODIPY) dyes through simple sonication reactions. Solids of BP composite materials are brightly fluorescent with 5 orders of magnitude increase of photoluminescence intensity compared with the pure solids of BP and BODIPY. 2D BP nanosheets with large specific surface area and lone pair electrons facilitate chemisorption of BODIPY by forming covalent interactions between P and B/N atoms, which not only passivates the surface of BP and eliminates the oxidation, but also prevents the aggregation caused quenching (ACQ) issue of BODIPY. Furtherly, the organic light-emitting diodes (OLEDs) based on the BP/chromophore composite luminescent materials were first successfully achieved, the electroluminescence spectra of which cover the full spectrum of red, green, and blue visible light. This work provides a brand-new approach to further design and development of high mobility and high luminous efficiency composite luminescent materials and devices based on BP.