The membrane modules of the water treatment system are faced costly damages; thereby executing pre-desalination units based on Nanofiltration (NF) could prevent these suffers, and improve the permeated water flux (PWF) and salt rejection (SR). Hence, we focused on the construction of a novel ternary-layer NF membrane through “electrospinning Polyvinylidene Fluoride (PVDF) (as bottom layer)”, “generating middle layer by electrospinning PVDF along with, the implementation cross-linking after electrospraying Sodium Alginate”, and “synthesizing Polyamide (as top layer) through interfacial polymerization”. More importantly, it anticipated that the Taguchi statistical method can expeditiously optimize the effects of Graphene Oxide nano-sheets (GOns) on water-dependent properties, such as PWF and SR. Astonishingly, the desalination capabilities significantly improved, when the top, middle, and bottom layers simultaneously had 1, 0.1, and 0.1 wt.% of GOns, respectively. Overall, comparing the performances between the optimized sample containing low-dosage and without GOns demonstrated the PWF ameliorated from 6.68 to 20.36 L/m2 h; also, the SR ability remained on an incremental basis as NaCl < MgCl2 < MgSO4 under 6 bar pressure. Manifestly, these authentic results denoted promising, innovative, and large-scaling insights when effectual PWF and SR be necessary.