Over the past two decades the Layer-by-Layer (LbL) assembly of multilayer thin films has witnessed an explosive growth. However, this has so far not been translated into numerous industrial applications mainly owing to the time-consuming multistep assembly procedure which was originally based on dipping of a substrate into a solution. More recently the use of spray-based approaches, both for planar films as well as for the construction of polymeric particles, has emerged. Here we highlight these recent advances that have the potential to move the LbL field forward.