An easy way of controlling pore sizes during the preparation of cellulose nanopapers using nanofibrillated cellulose and different solvents, such as water, ethanol and acetone, was applied in this study. A possible mathematical model is also presented, that describes the occuring processes, which model is based on simple probability theory computations taking the number of possible hydrogen bonds into consideration. This model allows the better understanding of the solvent dependence of pore formation on a molecular level. For the comparison of the effects of solvents two different series of cellulose nanopapers were prepared. In the cases of both series, an aqueous nanofibrillated cellulose suspension was used for the fabrication of nanopapers, and different solvents were used for their modification. Based on scanning electron microscopy images and mercury intrusion porosimetry data it has been concluded, that using different solvents was a crucial point in controlling pore sizes. A theory about the swelling effects, as well as the formation and decomposition of nanofibrillated cellulose aggregates based on the hydrogen bonding abilities of the solvents, was proposed and proven in this paper. As-prepared nanocellulose papers can be excellent candidates for further applications as support materials (e.g., virus filtration).