Products are manufactured as printed electronics through electro-conductive ink having properties suitable for flexible substrates. As printing process conditions affect the quality of the electronic properties of the final devices, it is essential to understand how the parameters of each process affect print quality. Spray printing, one of several printing processes, suits flexible large-area substrates and continuous processes with a uniform layer for electro-conductive aqueous ink. This study adopted the spray printing process for cellulose nanofiber (CNF)/carbon nanotube (CNT) composite conductive printing. Five spray parameters (nozzle diameter, spray speed, amount of sprayed ink, distance of nozzle to substrate, and nozzle pressure) were chosen to investigate the effects between process parameters and electrical properties relating to the morphology of the printing products. This study observed the controlling morphology through parameter adjustment and confirmed how it affects the final electrical conductivity. It means that the quality of the electronic properties can be modified by adjusting several spray process parameters.