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2D nanosheets produced using liquid phase exfoliation method offers scalable and cost effective routes to optoelectronics devices. But this technique sometimes yields high defect, low stability, and compromised electronic properties. In this work, we employed an innovative approach that improved the existing liquid phase exfoliation method for fabricating MoS2/graphene heterostructure-based photodetector with enhanced optoelectronic properties. This technique involves hydrothermally treating MoS2 before dispersing it in a carefully chosen and environmentally friendly IPA/water solvent for ultrasonication exfoliation through an optomechanical approach. Thereafter, heterostructure nanosheets of MoS2 and graphene were formed through sequential deposition technique for the fabrication of vertical heterojunctions. Furthermore, we achieved a vertically stacked MoS2/graphene photodetector and a bare MoS2 photodetector. The MoS2/graphene hybrid nanosheets were characterized using spectroscopic and microscopic techniques. The results obtained show the size of the nanosheets is between 350 and 500 nm on average, and their thickness is less than or equal to 5 nm, and high crystallinity in the 2H semiconducting phase. The photocurrent, photoresponsivity, external quantum efficiency (EQE), and specific detectivity of MoS2/graphene heterostructure at 4 V bias voltage and 650 nm illumination wavelength were 3.55 μA, 39.44 mA/W, 7.54 %, and 2.02 × 1010 Jones, respectively, and that of MoS2 photodetector are 0.55 μA, 6.11 mA/W, 1.16 %, and 3.4 × 109 Jones. The results presented indicate that the photoresponse performances of the as-prepared MoS2/graphene were greatly improved (about 7-fold) compared to the photoresponse of the sole MoS2. Again, the MoS2/graphene heterostructure fabricated in this work show better optoelectronic characteristics as compared to the similar heterostructure prepared using the conventional solution processed method. The results provide a modest, inexpensive, and efficient method to fabricate heterojunctions with improved optoelectronic performance.