In this work, a novel kind of solar cell based on the N-CQDs/MoS2 (0D/2D) quantum dimensional heterostructure has been fabricated using a two-dimensional (2D) MoS2 ultrathin layer and zero-dimensional (0D) Nitrogen-doped carbon quantum dots (N-CQDs). The combination of N-CQDs and MoS2 offers good optical and electrical characteristics. The current-voltage (I–V) characteristics of the quantum dimensional heterostructure have been recorded in the dark and under the illumination of solar radiations. A significant current rectification ratio has been observed in dark I–V characteristics. Furthermore, a remarkable shift of −13.49 mA in the I–V curve is observed on the exposure to solar radiation. The fabricated quantum dimensional heterostructure exhibits a significant power conversion efficiency (η) of 4.06% and an open-circuit voltage of 0.83 V. The external quantum efficiency (EQE) spectra support the recorded photovoltaic performance of the heterostructure. The aforementioned results could be ascribed to the effective separation of photogenerated electron-hole pairs at the junction contact. The N-CQDs serve as an electron blocking layer, preventing additional carrier recombination at the metal electrode. Our findings show that N-CQDs/MoS2 heterostructure has a great potential in futuristic low-cost, non-toxic, and highly efficient solar cells for next-generation energy harvesting applications.