The spray coating process is implemented through the production of smooth Montmorillonite (MMT) -Cellulose nanofiber (CNF) composite functioning as a barrier material and base substrate for printed electronics. In this process, the effect of MMT loading into the cellulose nanofiber (CNF) suspension for producing nanocomposite is independent of the operation time. Throughout this investigation, the barrier, surface, and topography of the spray coated nanocomposites were investigated. The MMT content varied from 5 wt.% to 75 wt.% in the composites via spraying of 2 wt.% of CNF suspension. Three types of nanocomposites were prepared from cellulose nanofiber with the MMT category of closite Na++, closite Ca++ and closite 116. By varying the MMT content in the nanocomposite, the spray coating was more productive with the basis weight of nanocomposites ranging from ῀70 g/m 2 to ῀100g/m 2 with sheet thickness varying from ῀81.7µm to 135.8µm and independent of the operation time which was less than 1 min. The air permeance and water vapour permeability of the spray coated nanocomposites were investigated to confirm the green materials was infact barrier material. Aggregation of MMT clays on a further increase of MMT in nanocomposite resulted in the elevation of WVP. The composite has two unique surfaces, namely rough and smooth surfaces from metal side. Scanning electron microscopy (SEM) reveals the distribution of MMT on the surface, compactness and smoothness of the composite. The composites are flexible, demonstrate good uniformity and pigmentation as a result of an increase in MMT loading.Considering the barrier performance and surface roughness of nanocomposites, it can be used as packaging materials and as a base substrate for printed electronics. In comparsion, spray coating is a more efficient process for producing sustainable nanocomposites as alternative for synthetic plastics.