Interest in nanocellulose-based coatings for packaging applications has been growing due to their excellent oil and gas barrier properties combined with their sustainable, recyclable, biodegradable, and non-toxic nature. Coating of nanocellulose materials such as microfibrillated cellulose (MFC) on paper/paperboard is challenging compared to traditional paper coating materials due to excessively high viscosity and yield stress of MFC suspensions at rather low solids content, typically below 5%. Possessing large amounts of water and a distinct rheological behavior such suspensions set tough demands on the substrate to be coated. It is important to understand and quantify substrate requirements in order to coat these suspensions successfully and achieve a satisfactory coating quality. A custom-built slot geometry is used herein to enable coating of highly viscous MFC suspensions on different paper-based substrates in a roll-to-roll process. The impact of substrate properties, such as surface chemistry and surface energy, surface roughness and surface porosity, and water absorption capacity on MFC coatability and coating quality is reported. Coating adhesion to the substrate was quantified with surface strength testing of MFC coated substrates. Various techniques, such as Scanning Electron Microscopy, IGT print penetration tests, and air permeability tests were employed for measuring coating coverage and surface porosity. MFC coating was found to adhere best to a highly hydrophilic surface, whereas the most uniform and defect-free film at low coat weights was formed on a smooth surface. It was also found that the MFC coat weight needed for full coverage, and therefore potentially good barrier, needs to exceed the surface roughness volume of the substrate. Water absorption capacity of the substrate also determines the final MFC coating quality obtained. The results clearly highlight the role of paper-based substrate for successful and effective coating of the micro and nanocellulose suspension.