The photocatalytic solar-to-chemical energy conversion by direct utilizing the full spectrum of sunlight is attracting a great deal of current attention. Black phosphorus (BP), a “rising star” of post-graphene two-dimensional (2D) nanomaterial, holds a unique advantage for this purpose on account of its tunable direct-bandgap for broadband absorption. In this work, for the first time, we anchor BP quantum dots (BPQDs) of ∼ 4.2 nm in size onto molybdenum disulfide (MoS2) nanosheets of ∼ 3 nm in thickness to create 0D/2D nanohybrids with various BP contents (5–20 wt %) via a facile and cost-effective grinding and sonicating approach. The as-prepared BPQDs/MoS2 nanohybrids show enhanced photocatalytic performance towards methylene orange degradation in water under visible− and near−infrared (NIR) light illumination, respectively. Notably, 10 wt% BPQDs/MoS2 nanohybrids with cyclability achieve the highest NIR−driven photoactivity (3 × 10−2 min−1), which is approximately 13 and 27 folds higher than that of individual BPQDs and MoS2, respectively. We demonstrate that the enhanced light absorption, the type−II band alignment, and the interfacial bonding and the spatial charge separation between well-dispersed BPQDs and MoS2 synergetically enhance the photoactivity and photostability. This study may open avenues to create BP-based heterostructures functional in solar-to-chemical energy conversion and beyond.